According to the official records of the Orbiting Frog Otolith mission, this occurred on November 9, 1970, when a Scout rocket launched from Wallops Island, Virginia, with the two frogs into low Earth orbit for six days, as part of an experiment studying the effects of zero-gravity on balance. The frogs rode inside a water-filled canister wired with sensors, part of an unmanned satellite that had no plans to ever return to Earth.
Meet Pierre and Tee-Nom