Despite impressing club management with his coaching on the training field, Defoe revealed that off-the-pitch circumstances made it impossible for him to remain in his post.
Writing in a post on his personal Instagram account, the former Tottenham Hotspur star delivered his farewell message: "Unfortunately, circumstances have ultimately made it impossible for me to continue in the position.
"I am extremely proud of the work undertaken during my time at the club and genuinely felt that we were building something special.
"My time at Woking FC has been an eye-opening managerial experience and one that will undoubtedly make me stronger for the next challenge in my career."