Defoe worked a number of youth sides including the U17 to U21 squads at Spurs where he has proven to be an inspiration to many of the young players.
This role came after the ex-England striker had undertaken coaching duties as part of Steven Gerrard’s staff at Rangers during the final few years of his successful career.
The Premier League icon spoke on Instagram about how he loved his time at the club and now wants to switch careers.
“For the past two seasons I have thoroughly enjoyed my coaching time at THFC.
“Today I leave this incredible club, and I want to say thank you to all the amazing people in the building who have helped me learn and grow.
“It has been a pleasure to achieve so much at Spurs including reaching UEFA A coaching status which was always an ambition of mine following my playing career.
“Spurs will always hold a special place in my heart and the fans already know how much the club means to me.
“However, now is the right time for me to move on and shape the rest of my coaching and managerial career, nevertheless I will forever remember my time at Spurs fondly.
“All great journeys eventually come to an end and I wish everyone at the club nothing but the best for the coming season and the future.
“Until next time.”