The ex-Chelsea and Manchester United midfielder suffered a cardiac arrest on Saturday and was admitted to St George's Hospital, where he had been put in an induced coma.
"It is with great sadness we announce that Raymond Colin Wilkins passed away this morning," his family said in a statement on the St George's website.
"We would like to thank St George's staff for the amazing work they have done to care for our beloved Ray.
"We would also like to say thank you for the many goodwill messages we have received from Ray’s friends, colleagues, and members of the public."
Wilkins won 84 caps for England between 1976 and 1986.
He also played more than 150 times for each of Chelsea, Manchester United and Queen's Park Rangers, with shorter spells abroad for AC Milan and Paris St Germain."Everybody associated with Chelsea Football Club is devastated to learn of the passing of our former player, captain and assistant coach, Ray Wilkins. Rest in peace, Ray, you will be dreadfully missed," the west London club said in a tweet.
In a 20-year coaching career Wilkins also managed QPR, Fulham and the Jordan national team. He was assistant manager in two spells at Chelsea where he started out as a player.
FA CUP WINNER
Wilkins came through the youth ranks at Chelsea and made his senior debut aged 17 against Norwich City in 1973.
He joined United after Chelsea were relegated in the 1978-79 season and won the FA Cup with the Old Trafford club in 1983.
Wilkins made his England debut aged 20 against Italy in a tournament in the United States and was a fixture in the England side for the next decade, captaining the team 10 times.
England striker Gary Lineker wrote on Twitter that no team mate was as "helpful and supportive" as Wilkins.
"Deeply saddened to hear that Ray Wilkins has passed away," Lineker said. "A wonderful footballer and a delightful man. It was a pleasure to have played alongside him with England."
AC Milan, for whom Wilkins made more than 70 appearances between 1984 and 1987, will honour him later on Wednesday when they face city rivals Inter in a Serie A match.
"Goodbye Ray, you will be missed: tonight we're gonna fight like you taught us!" Milan said in a tweet.
Former Manchester United defender Rio Ferdinand also offered his condolences and paid tribute to Wilkins the man and player.
"Always so humble and softly spoken whenever I saw him. Genuine lovely guy," Ferdinand said in a tweet. "Watched him... at Loftus Road many times for QPR. What a great passer and teacher of the game for any young kids who watched him."
Wilkins is survived by his wife Jackie and their two children and grandchildren.
Sumber Former England captain Wilkins dies aged 61