Bosworth was cast as reporter Lois Lane in Bryan Singer's superhero film Superman Returns (2006). She starred along with her Beyond the Sea co-star Kevin Spacey as Lex Luthor, as well as newcomer Brandon Routh as Superman. The film was a box office success and received mostly positive reviews. Bosworth's performance however, was not well received among critics; Anthony Lane of The New Yorker noted, "The new Lois Lane, Kate Bosworth, is not a patch on Margot Kidder, or, for that matter, on Teri Hatcher, in the TV series." San Francisco Chronicle film critic Mick LaSalle felt that Bosworth, at the age of 22 years, was too young to portray Lois Lane, and the climax did not "match the potential of the tiring 154 minute long film". Although Bosworth's performance was ambivalently received, she herself loved the experience of working on the movie. As she told Teen Vogue in August 2006, "You know how you have an experience, a time in your life when you feel you've come into your own? When you grow up a bit, and think, Now I get it? [...] That's how I feel. I feel a little bit more complete." The movie grossed $52 million during its opening weekend in North America and went on to earn $391 million worldwide.
In 2006, she optioned the film rights to Catherine Hanrahan's novel Lost Girls and Love Hotels and was set to produce the project alongside filmmaker Nadia Connors. As of 2016, the project was at a standstill. In 2010, she starred in The Warrior's Way, which was shot in New Zealand alongside Korean actor Jang Dong-gun and Geoffrey Rush. The film was one of 2010's biggest box office flops, grossing only slightly more than $11,000,000 worldwide, but costing $42 million. She has said about her roles, "I just don't do comfort zones."