The duo have left Fold after a four-year tenure at The Elliot Scott Group Stadium.
The Mundays have overseen many landmark moments at the club.
Fold stepped into senior football for the first time, having secured promotion to Southern Combination Football League Division 1, in 2017-18.
The Mundays and Alfold then lifted the Division 1 title, and earned promotion to the Premier Division, at the first time of asking a season later.
Fold also played in the FA Cup for the first time in the club's history in 2020-21.
The Surrey outfit thumped Shoreham 9-1 in the extra preliminary round before they were beaten on penalties by Erith & Belvedere a round later.
A joint-statement from Jack and Matt on Twitter said: "After four incredible years as manager at Alfold FC it's with a heavy heart that we have decided to step down from our roles.
"This was one of the toughest decisions to make, it's become a huge part of our life from the first day we took over.
"We've enjoyed many highs at the club. From our first promotion in our debut season... to entering the FA Cup for the first time in the club's history.
"We've met some great people and have shared some brilliant battles and rivalries from the likes of Roffey and Rustington to Steyning and Loxwood.
"Although we haven't always covered ourselves in glory at times, we have huge respect for every other manager and coach we've come up against as we understand the challenges of being a football manager.
"This is why we've taken the tough decision to step away from football.
"We are both at a point in our lives where we want to focus on our families.
"We'd like to take this opportunity to thank everyone involved with the football club, past and present, and most importantly every player that has put on an Alfold shirt during our time as managers.
"We wish nothing but success and will always continue to support the club. Up the Fold."