Film and television
In 2016, Croft appeared in the ITV and Fox series Houdini and Doyle and the Sky Atlantic and Showtime series Penny Dreadful. Croft rose to prominence portraying the role of a young Eddard Stark (portrayed by Sean Bean as an adult and Robert Aramayo as a young adult) in the sixth series of the HBO series Game of Thrones.
Croft made his feature film debut in 2017 as a Young David Logan in The Hippopotamus. He appeared in the 2019 films Music, War and Love and Horrible Histories: The Movie – Rotten Romans as Young Robert Pulaski and Atti respectively, the latter of which earned him a BAFTA Children's Award nomination in the Young Performer category.
Croft voiced Peter van Daan in the animated fantasy film Where Is Anne Frank, which premiered at the 2021 Cannes Film Festival. He lent his voice to Volume II of the Netflix animated anthology Love, Death & Robots in the episode "Ice". Croft and Ty Tennant were cast as the Dead Boy Detectives Charles Rowland and Edwin Paine respectively in series 3 of the DC Universe series Doom Patrol.
In April 2021, it was announced Croft would play Ben Hope in the 2022 Netflix series Heartstopper, an adaptation of the webcomic and graphic novel of the same name by Alice Oseman. Later that year, he was part of the cast of the horror-fantasy film Dampyr released in Italy on 28 October 2022. Croft co-starred with Charithra Chandran in the young adult romantic comedy How to Date Billy Walsh for Amazon Prime.
In August 2023, it was confirmed that Croft would not be returning for the third series of Heartstopper as Ben Hope, given his character's storyline had finished in the second series's seventh episode.
In November 2023, it was announced Croft would star in the film Get Away (originally titled Svalta) with Nick Frost and Aisling Bea. The same month, Croft joined the cast of the BBC crime drama series Dope Girls.
Croft is appearing on the second series of The Celebrity Traitors, which began in October 2026.