Liverpool's Steven Gerrard (Photo: Reuters)
Gerrard, 34, led the national team at the World Cup where England bowed out in the group stage and the Liverpool midfielder said he had "agonised" over the decision since returning from Brazil.
"This has been a very difficult decision, one of the toughest I've had to make in my career," Gerrard told the Football Association's FATV.
"I have enjoyed every minute of representing my country and it is a sad day for me knowing that I won't pull on the England shirt again.
"To ensure I can keep playing to a high level and giving everything to Liverpool Football Club I believe this is the right decision, and having Champions League football back at Anfield is another big factor in my decision," he added.
Gerrard, who made his international debut against Ukraine in 2000, trails just Peter Shilton (125) and David Beckham (115) on England's all-time caps list.
He appeared at three World Cup finals as well as three European championships and scored 21 goals for the Three Lions. He captained England in Brazil and at Euro 2012.
England coach Roy Hodgson paid tribute to Gerrard, saying: "While I'm disappointed in the decision, I can entirely understand Steven's situation and can have no complaints given the incredible service he has given to his country."
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