Brad Garlinghouse has been named president of internet and mobile communications, a role with global responsibilities for expanding the reach of email and instant messaging.
He reports to AOL's chairman and chief executive Tim Armstrong, who took up the role in April.
AOL is currently in the process of demerging from Time Warner and will become a separately listed company once again, having merged with the publishing giant in 2001.
Garlinghouse worked for Yahoo! for six years, running its email operations. He became famous after an internal memo he wrote, known as 'The Peanut Butter Manifesto' was leaked.
In it, he said that Yahoo! was spreading itself too thinly and lacked a cohesive strategy. He also said the company was "reactive instead of charting an unwavering course".
He left Yahoo! at the end of 2008 and has been working as an adviser to private equity firm Silver Lake Partners.
Garlinghouse's appointment comes following a 100-day consultation instigated by Armstrong, who joined AOL in April.
It has resulted in the identification of five areas of focus for AOL -- communications, content, advertising, local and mapping and AOL Ventures, the venture capital arm.
In his new role, Garlinghouse will also serve as West Coast lead for AOL Ventures.
Armstrong said: "In addition to leading our efforts to grow our communications products, Brad will be bringing his global leadership and business experience as a key member of our company's executive leadership team.
"He will also be a major force for AOL in Silicon Valley, working to expand our presence there and in the tech community in general."
Garlinghouse said it was a "tremendous opportunity to join AOL at this pivotal moment in its history".
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