After appearing briefly in Cameron Crowe's Oscar winning film Almost Famous, Baruchel won the role of Steven Karp on Judd Apatow's acclaimed yet short-lived television series Undeclared, where he starred alongside Seth Rogen, Carla Gallo, Charlie Hunnam, and Monica Keena.

Baruchel then starred in Nemesis Game and Fetching Cody, before appearing opposite Don Johnson on the WB's Just Legal in 2005, and guest-starring on the CBS drama Numb3rs in 2006.

Baruchel appeared in the films Knocked Up (which reunited him with Judd Apatow, Jason Segel, and Seth Rogen), I'm Reed Fish, Just Buried, and the Ben Stiller-directed Tropic Thunder, alongside Jack Black, Nick Nolte, Steve Coogan, and Robert Downey Jr.

In 2010, Baruchel starred in the films The Trotsky, DreamWorks' She's Out of My League (opposite Alice Eve),[14] and the live-action Disney adaptation of The Sorcerer's Apprentice.

Also in 2010, he played two supporting characters in the Canadian comedy series The Drunk and On Drugs Happy Fun Time Hour.

[17] Baruchel also appeared in the 2010 Adidas Originals ad campaign, "Cantina", in conjunction with the FIFA World Cup and in video clips for Canadian prog-rockers Rush's 2012–13 Clockwork Angels tour.

In the summer of 2013, he starred in the hit apocalyptic comedy This Is the End and in 2014, he appeared in the RoboCop remake and reprised his role as Hiccup in How to Train Your Dragon 2.

The book explored his love of the Montreal Canadiens with anecdotes, childhood memories, and heartfelt tales about his life as a fan of the team.

[22] In the same year, Baruchel and his wife, Rebecca-Jo Dunham, both appeared in the music video for "Ouch", the lead single from The Tragically Hip's archival EP Saskadelphia.

Baruchel, as host, met with scientists and other experts to discuss the feasibility of the risks and the potential solutions and innovations to counter the issues.

[33][34] Baruchel has several tattoos among which, a Celtic cross on his upper right arm to honour his Irish heritage,[35] and a red maple leaf on his left pectoral.