Ross, named to the job in October 2009, was never able to duplicate the success he enjoyed as president of the Disney Channel, where he was credited with creating monster franchises that included "High School Musical" and "Hannah Montana."
"I no longer believe that the Chairman role is the right professional fit for me," Ross told his staff in an email.
Disney will not immediately name a new head for its studio, a source familiar with the matter said.
In a statement, Disney CEO Bob Iger said: "For more than a decade, Rich Ross' creative instincts, business acumen and personal integrity have driven results in key businesses for Disney. ... I appreciate his countless contributions throughout his entire career at Disney and expect he will have tremendous success in whatever he chooses to do next."
As the company's studio chief, Ross approved production of "John Carter," an expensive science-fiction epic whose development started years earlier. The film's costs eventually ballooned to more than $250 million.
Disney said in March it expected the film to lose about $200 million and to saddle its studio with $80 million to $120 million in operating losses.
Ross joined Disney Channel in 1996 as a programming and production executive and was promoted to president of the cable channel in 2004. His success at the Disney Channel made him a rising star in the company and eventually led to his being hand-picked by Iger to replace long-time chairman Dick Cook, whom Iger forced out, as head of its film division.
Two weeks before his departure, Ross hosted a lavish Hollywood premiere for "The Avengers," a big-budget special effects film featuring action stars from Disney's Marvel subsidiary. The film is expected to be one of the summer's biggest hits.
Disney shares were up 67 cents, or 1.6 percent, at $42.75 in midday trading on Friday.
(Reporting By Ronald Grover; editing by Peter Lauria, Lisa Von Ahn and Andre Grenon)
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