Redknapp, who was tipped for the England manager's job before Roy Hodgson's appointment, had a year remaining on his contract at the club.
But amid reports of failing to agree terms on a new deal with the club's chairman Daniel Levy, it has now been confirmed Redknapp has left.
"This is not a decision the Board and I have taken lightly," Levy said in a statement on the club's website.
"Harry arrived at the Club at a time when his experience and approach was exactly what was needed. This decision in no way detracts from the excellent work Harry has done during his time with the Club and I should like to thank him for his achievements and contribution.
"Harry will always be welcome at the Lane."
The news comes less than two days after Redknapp was forced to issue a statement denying he had left the club, following claims on social media sites that he had quit.
He joined Spurs from Portsmouth in 2008, and guided them to their first ever Champions League campaign in 2010. Last season they finished fourth in the English Premier League, but missed out on a return to the Champions League after Chelsea won the competition.
The 65-year-old has been linked in the past with managerial positions in the UAE Pro League.
Current Everton manager David Moyes has been installed as the favourite to replace Redknapp in the White Hart Lane dugout.
"I have thoroughly enjoyed my time at Spurs and am proud of my achievements," Redknapp said on Spurs' website.
"I have had a fantastic four years with the Club, at times the football has been breathtaking. I am sad to be leaving but wish to thank the players, staff and fans for their terrific support during my time there."
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