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In 2008, Russell Brand shot to fame in the U.S. when he was seen as the rocker Aldous Snow in the Judd Apatow-produced comedy Forgetting Sarah Marshall. The film, which was written by and starred Jason Segel, grossed $63 million at the domestic box office. That same year, Brand also starred in the Disney film Bedtime Stories, which also featured Adam Sandler and Keri Russell. It was in September 2008 that Brand cemented his fame in the U.S., when he hosted the MTV Video Music Awards (VMA).

The year 2009 saw the U.S. release of Brand's writing debut, "My Booky Wook: A Memoir of Sex, Drugs and Stand-Up." The autobiography, already a huge success in the United Kingdom, went on to stay on The New York Times best-seller list for five weeks in a row. In continuation of his stand-up tour in the U.S., Brand's third live DVD was released after originally airing on Comedy Central. The year 2009 ended on an even brighter note for Brand when he assumed the role as host of the MTV Video Music Awards for the second year in a row and garnered the biggest VMA audience since 2004, with nearly nine million viewers.

The year 2010 was a busy year for Brand with the release of the hit comedy Get Him to the Greek in June. Reunited with producer Judd Apatow, Brand starred, opposite Jonah Hill, and reprised his iconic role as Aldous Snow. In July, Brand also lent his voice to the role of Dr. Nefario in the hit animated feature film Despicable Me, which included the vocal talents of Steve Carell and Jason Segel. Brand also starred, alongside Helen Mirren, in Julie Taymor's adaptation of The Tempest. His upcoming roles include the title character in the remake of Arthur.

In addition to acting, Brand released his second book, Booky Wook 2: This Time It's Personal.