Television
Kroll's first significant career success came when he co-starred in the ABC sitcom Cavemen, based on the Geico insurance TV commercial characters. Although the show was cancelled after seven episodes, he called his role "the most important experience of my professional career". He went on to VH1's Best Week Ever, and to guest-starring roles on Parks and Recreation, Community, Unbreakable Kimmy Schmidt, and New Girl. He made appearances on numerous Comedy Central series such as Reno 911!, John Oliver's New York Stand Up Show, and The Benson Interruption, both performing as himself and in character.
Kroll had a starring role as Rodney Ruxin in the FXX comedy series The League, which aired October 29, 2009, to December 9, 2015. Concurrently, he created and starred in his own Comedy Central sketch series, Kroll Show, which aired January 16, 2013, to March 24, 2015. Kroll had a recurring role on Childrens Hospital on Adult Swim. His voice work includes the character Stu on the HBO animated series The Life & Times of Tim, Andrew LeGustambos in the animated Fox comedy series Sit Down, Shut Up, and Reuben Grinder in the PBS Kids GO! series WordGirl. Kroll was one of the roasters on the Comedy Central Roast of James Franco.
In 2017, Kroll co-created, wrote, and starred in Big Mouth, an animated television show on Netflix. The show features the experiences of a group of 7th graders in the throes of puberty. Two of the main characters are based on, and named after, Kroll and his best friend from childhood, Andrew Goldberg. Kroll plays Nick, as well as Coach Steve, Maurice the Hormone Monster, Lola, Rick the Hormone Monster, the Jansen twins and Lady Liberty, in addition to several further minor and one-off characters. The show's success led its creators – Kroll, Andrew Goldberg, Mark Levin and Jennifer Flackett – to form the production company Brutus Pink, which works with Titmouse, Inc. to produce other shows for Netflix like the spin-off Human Resources, as well as the series Mating Season.