"I have played 106 times for Germany. There will not be another time," the 31-year-old Real Madrid star wrote on Twitter.
"I had already made the decision to retire after this tournament," he added, referring to the European championships which ended for the Germans when they lost 2-0 to England in the last 16 on Tuesday at Wembley.
Kroos said he planned in the next years to place his "full concentration" on Real Madrid.
"I would also like to be there more as husband and father for my wife and children," he wrote.
"Due to the (international) breaks that I will get in the future, I believe that I can recharge my battery better," he added.
Thanking supporters and critics alike, Kroos also had special words for Joachim Loew, who bowed out as national coach on Tuesday following 15 years in the job.
"He made me a national team player and a world champion. He trusted me. We wrote a success story together."
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