Harlequins' Care played his 101st and final England game in this month's Six Nations loss against France - 16 years after making his debut in 2008.
"Playing for England has meant the world," Care said on social media.
"It's meant an awful lot for me to represent this country.
"I've never taken it for granted, I would never take it for granted," he added.
Care became the sixth England men's player to reach the century during the narrow Six Nations victory over Ireland at Twickenham on March 9th.
He had spent four years away from the international scene after being dropped in 2018 returning during last year's Six Nations.
Care played six games during England's run to third place in the 2023 Rugby World Cup.
"All good things do have to come to an end at some point," Care said.
"I feel the time is right now to pass the baton on.
"I'm going to miss it but I feel the time is right to step away and be with my family. What a ride it's been," he added.
