The venture, announced at E3 2012, will bring PlayStation 3 and Xbox 360 titles to Samsung's Smart Hub devices over the air.
"Samsung is excited to deliver this revolutionary gaming experience that takes advantage of all the benefits of cloud-computing, all on the central screen of the home," said Samsung vice president Kyung-shik Lee.
Gaikai entered a similar partnership with LG earlier this year to bring its gaming service to the firm's smart TVs. A prototype version of the platform was showcased at the CES 2012 show in Las Vegas.
Samsung will pay Gaikai a fee for the use of its technology and pursue separate deals with gaming companies to bring their software to its devices.
Gaikai's chief executive David Perry said: "Together, we will turn Samsung Smart TVs into a console-like experience capable of delivering the best-selling video games and other content instantly to consumers - no downloads, no extra hardware, no trips to the store."
Sony has been linked with a takeover bid for Gaikai, a move that could see its library of PSOne and PS2 games released for its current formats over the air.
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