Athletes and trialists taking part in the event will use the device's near field communication (NFC) technology to purchase goods and services around London, and gain access to the Olympic Village through the Visa payWave app.
Visa says that purchases exceeding £20 will require a password to authorise for security purposes. The application, which could be rolled out on a wider scale after the games, also tracks sending and purchase history.
Sandra Alzetta, senior vice president of mobile with Vis Europe, said: "Mobile technology has long been a revolutionary force in our lives and NFC-enabled devices such as the Galaxy S3 will fundamentally change the way we pay.
"The future is mobile and cash usage will only continue to decline as people use their mobile devices to manage their money, shop and pay.
"This summer our partnership with Samsung will showcase all the advantages of the future of payments: security, convenience, speed and flexibility being forefront among them,"
The Samsung Galaxy S3, unveiled at a press event in London last week, arrives in stores on May 29.