Established actress (2013–2018)
Although Samantha often portrayed strong character roles in her early films, post-2012, she has appeared increasingly in big-budget, hero-oriented films, which have comparatively smaller scope for actresses. Samantha next appeared in the Telugu multi-starrer film, Seethamma Vakitlo Sirimalle Chettu (2013) alongside Venkatesh and Mahesh Babu, which received positive reviews and was commercially successful. Though her role was comparatively minuscule to her co-stars, IBN Live noted it was "good to see Samantha shed her glamorous side and welcome performance-oriented roles, which she only handles with deftness and ease". The romantic comedy Jabardasth (2013) alongside Siddharth, in which she portrayed a wedding planner, became a commercial failure, though critics noted Samantha is "getting better by the day and it's a delight to watch her on screen". Samantha then starred alongside Pawan Kalyan in the family drama, Attarintiki Daredi (2013), which emerged as the highest-grossing Telugu film upon release. A critic from Rediff.com noted Samantha "exudes confidence even though she has limited screen time and nothing much to do", and her performance saw her win Best Actress recognition at the SIIMA Awards and the Santosham Film Awards, in addition to her fourth nomination for the Filmfare Award for Best Actress – Telugu. Her final release of 2013 was in the unsuccessful Telugu masala film Ramayya Vasthavayya, where she had a small role, with a critic noting "we have seen Samantha in better roles and better films." Samantha was involved in a spat with actor Mahesh Babu and his fans after she criticized a promotional poster for the Telugu film, 1: Nenokkadine (2014) in December 2013; she had tweeted that the way actress Kriti Sanon was depicted as crawling behind Mahesh Babu was "deeply regressive".
The year 2014 saw Samantha appear in six films and make a return to the Tamil film industry. Her first release saw Samantha portray a dual role in the family drama film Manam (2014), where she featured alongside several members of the Akkineni film family. Featuring as a young mother and a college student in two different time eras, Samantha received positive reviews for her work, with the critic from Sify saying "she excels" and The Hindu's reviewer noting that she "emotes well and easily shifts between the roles." Her performance fetched Samantha her fifth nomination for the Filmfare Award for Best Actress – Telugu, while she won Best Actress (Critics) at the SIIMA Awards. Samantha subsequently featured alongside Naga Chaitanya again in the long-delayed Autonagar Surya (2014), before playing different minuscule roles in the Telugu action masala films Alludu Seenu (2014) and Rabhasa (2014). Critics lamented that she "signed up to be a glam doll" for the ventures. She has "previously shown us she is capable of doing much more, but of late, seems to be stuck with doing similar roles that require her to be an attractive prop." Samantha later revealed that she solely worked on Alludu Seenu as a favor to producer Bellamkonda Suresh, who had helped her delay the making of Jabardasth during her health problems.
Samantha worked simultaneously on two big-budget Tamil films in early 2014, working with industry-leading actors and directors. N. Lingusamy's gangster masala film Anjaan (2014) opposite Suriya, received negative reviews and performed poorly at the box office. Portraying a small role, critics panned her character in the film, stating Samantha "gamely performs the requisite crazy girl duties". Her other release, AR Murugadoss's action drama Kaththi (2014) opposite Vijay won predominantly positive reviews and became the most profitable Tamil film of 2014. Again, reviewers criticised her character stating "all she had to do in the film is smile and look pretty", while The Hindu remarked she played "an emoticon" and "that covers her contribution to the proceedings". She received her second nomination for the Filmfare Award for Best Actress – Tamil for her performance in Kaththi. She subsequently featured in the Telugu film S/O Satyamurthy with Allu Arjun, as a part of another hero-oriented film, though critics noted she "enacts her part with grace" and that she "plays her role well".
She then featured in her second dual role as a part of Vijay Milton's road film, 10 Endrathukulla (2015), where she appeared alongside Vikram. She sported a different rural look for the role and her performance won mixed reviews, with a critic noting "Samantha doesn't make much of an impact in the film except towards the end." Like Anjaan and Kaththi, critics lamented her role as a clumsy girl, with Sify.com stating "beyond a point Samantha's character is plainly annoying". Samantha subsequently won positive reviews for her role and performance in Velraj's Thanga Magan, where she featured opposite Dhanush. Portraying a homely role of a wife for the first time in Tamil films, the actress noted it would be the first of many such performance-oriented roles, as she looked to move away from being typecast in charming characters. A critic from Sify.com labelled her performance as "impressive", while DNA.com stated Samantha "has given a very subdued and mature performance sans drama". Likewise, a reviewer from Silverscreen, suggested that she "delivers a performance that stands head and shoulders above her work in previous films".
Samantha's first release of 2016 was in the Tamil romantic drama film Bangalore Naatkal, where she made a guest appearance and reprised Nithya Menen's minor role from the film's Malayalam original. She then portrayed the lead female role in Atlee's Theri, and featured alongside Vijay for the second time. Her performance received positive reviews, with a critic from DNA India stating "Samantha looks pretty as always" and that "she has done an incredible job in dubbing with a range of emotions in her numerous shades – doctor, lover, mother – and she shines". Likewise, Behindwoods.com stated that Theri "could be one of Samantha's best roles; she plays a doctor and has given out a soulful performance". The film went on to become of the most profitable Tamil films of all time, upon release, and ended a barren spell for the actress in Tamil cinema, by becoming her first commercially successful film in Tamil cinema since Kaththi (2014). Samantha then worked for a second time with director Vikram Kumar and Suriya in the critically acclaimed fantasy film 24. Featuring as the love interest of the film's lead character, Samantha won praise from critics for her small role in the film, with Sify.com stating that the actress "does well in the comedy scenes". The film also performed well at the box office, with The Hindu stating she was "at the top of the film industry", following her back-to-back commercial successes. She received two nominations for the Filmfare Award for Best Actress – Tamil for her performances in Theri and 24 respectively.
Samantha also featured in three high-profile Telugu films during 2016; Although Srikanth Addala's family drama Brahmotsavam opposite Mahesh Babu was a box office failure, her role in Trivikram Srinivas's romantic comedy, A Aa alongside Nithiin, won her high critical acclaim and commercial success. Portraying Anasuya Ramalingam, a naive girl trying to escape from her mother's controlling behavior, Samantha received highly positive reviews for her character portrayal. A critic from The New Indian Express noted "A Aa undoubtedly is Samantha's film" and that "right from her first frame till the last, she delivers a stellar performance and shows what she can do if given ample screen time", adding that she was "a joy to watch". Likewise, a reviewer from The Hindu noted "Samantha, after a long time, gets enough screen time and scope to shine", stating "she's vulnerable as a 23-year-old reeling in her mother's shadow and can also play the high maintenance, stubborn girl with ease", while concluding "this is a role she can be proud of". Similarly Bollywoodlife.com noted her "earnest performance was the life and soul of the romantic comedy", while DNA India's critic cited that "Samantha and Nithiin's performances in this movie will be what people would rave about for days to come". The film also performed well at the box office, doing excellent business for a Telugu film released in the United States. Her performance fetched her several awards, including the Filmfare Award for Best Actress – Telugu, her second win in the category. She then featured in the commercially successful action film Janatha Garage directed by Koratala Siva, with a critic noting despite "a limited role, she gives a nice performance". She then portrayed the lead female role in Atlee's Mersal, and featured alongside Vijay for the third time and her performance received positive reviews and the film became one of the highest grossing Tamil films of 2017 and was a blockbuster at the box office. Mersal went on to join the coveted ₹200 crore club.
In 2018, she starred in Rangasthalam which went on to become one of the highest grossing Telugu films. The Tamil action thriller Irumbu Thirai in which she starred opposite Vishal and the Telugu biographical drama Mahanati were successful at the box-office and each had a run of 100 days at the box office. Her performances in Rangasthalam and Mahanati were highly praised, and she earned her seventh Best Actress – Telugu nomination for the former and her first Best Supporting Actress – Telugu nomination for the latter at the Filmfare Awards. Mridula R from The News Minute noted her critically acclaimed film U Turn as a curiosity-generating script that provides her with the ultimate screen presence since the story begins with her and she finds it ends, rather that not being shaking a leg in Anjaan, Brindavanam, Kaththi and Attarintiki Daredi or being glam doll or having out-of-scope performances overshadowed in Dookudu, S/O Satyamurthy, Brahmotsavam, Theri and Mersal.