Harris was part of the Horsham team that achieved promotion to the Isthmian Premier via the play-offs in 2018-19.
The midfielder also played a key role in the Hornets’ fairytale adventure to the first round of this season's FA Cup and their run to Velocity Trophy glory.
He appeared 142 times for Horsham and scored 26 goals, many of them spectacular long-range efforts.
Posting on Twitter, Harris said: "My time at @HorshamFC has come to an end! What a journey it has been and truly the best 5 years!
"Want to say a big thank you to the @LardyArmy and all the fans who have been amazing since the start! Football must go on and onto the next chapter now!"
Harris becomes the fourth Hornet to exit the Camping World Community Stadium after the conclusion of the 2021-22 campaign.
Fellow fan favourites Steve Metcalf, Will Miles and Rob O'Toole have also chosen to leave the club.
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