2010–2012: Tron: Legacy and worldwide recognition
In 2010, Hedlund played Sam Flynn, the main protagonist in the science fiction / action film Tron: Legacy, acting alongside Jeff Bridges and Olivia Wilde. Hedlund won a "Darwinian casting process" which tested hundreds of actors, being chosen for having the "unique combination of intelligence, wit, humor, look and physicality" that the producers were looking for in Flynn's son. Hedlund trained hard to do his own stunts, which included jumping over cars and copious wire and harness work. The film was released on December 17, 2010, and directed by Joseph Kosinski. It is a sequel to the 1982 film Tron, whose director Steven Lisberger returned to produce. Like its predecessor, Tron: Legacy has also been described as a cult film. Hedlund was also considered by Disney to play Captain America / Steve Rogers in the Marvel Cinematic Universe, but had to abandon the project because his film schedule got in the way of Tron: Legacy.
Hedlund co-starred with Gwyneth Paltrow, Leighton Meester and his Friday Night Lights co-star, country musician Tim McGraw in the musical drama Country Strong, which was released on December 22, 2010. He recorded a number of songs for the film including "Chances Are" which appeared on Country Strong: Original Motion Picture Soundtrack. His performance was well received by critics. Noting voice similarities between Hedlund and Charlie Robison, Roughstock said "the best song on this album belongs to him" and Country Weekly wrote that of all the songs performed by actors in this film, his was "the most convincing". Six other songs, including a duet with Meester, were featured on a second soundtrack titled Country Strong: More Music from the Motion Picture.
On June 7, 2011, Hedlund was named "Man of the Year" at the Glamour Awards.
He also co-starred with Kristen Stewart, Sam Riley, Kirsten Dunst and Viggo Mortensen as Dean Moriarty in the 2012 adventure drama On the Road, produced by Francis Ford Coppola. The film was directed by Walter Salles and based on Jack Kerouac's novel of same name. Hedlund's performance in this film was praised by critics. In The Hollywood Reporter, veteran reviewer Todd McCarthy writing "Although the story is Sal / Kerouac's, the star part is Dean, and Hedlund has the allure for it; among the men here, he's the one you always watch, and the actor effectively catches the character's impulsive, thrill-seeking, risk-taking, responsibility-avoiding personality." Entertainment Weekly magazine's Owen Gleiberman wrote, "The best thing in the movie is Garrett Hedlund's performance as Dean Moriarty, whose hunger for life – avid, erotic, insatiable, destructive – kindles a fire that will light the way to a new era. Hedlund is as hunky as the young Brad Pitt, and like Pitt, he's a wily, change-up actor".
That same year, he was an advertising and catwalk model for the Italian fashion firm Prada.
Hedlund was cast as Kaneda Shotaro in the live-action version of Akira but production of the film was cancelled. Hedlund reportedly turned down the roles of Christian Grey in the film adaptation of E. L. James' best-selling novel Fifty Shades of Grey and Finnick Odair in the sequel to the dystopian science fiction / adventure film The Hunger Games titled The Hunger Games: Catching Fire.