The former I'm A Celebity... star was placed in the bottom two alongside McFly's Danny Jones after the public vote.
The four judges were then asked to decide which singer was to remain in the competition. After some deliberation, all four selected Jones.
Following confirmation of his exit, Osmond told host Alan Titchmarsh that he enjoyed his stint on the show but was looking forward to returning home to his family. "I've had a blast!" he said.
Popstar To Operastar continues next Friday at 9pm on ITV1.
> Click here for our video interview with Jimmy Osmond