Originally founded as a Dutch team with the name Mooroolbark United Soccer Club in 1962, Mooroolbark's backing changed to a British influenced club in its formative years.

The club's claim to fame is as Victoria's (and Australia's) first national sporting club side. Mooroolbark enabled the National Soccer League to proceed, breaking the deadlock which was then in force between the budding national league and clubs from Victoria, whom the Victorian Soccer Federation had forbidden to join the competition. When Mooroolbark joined the NSL, officially as its first entrant, soon three other Victorian clubs, South Melbourne, Heidelberg United and Footscray JUST also joined, enabling the competition to go ahead.

Mooroolbark's stay in the NSL however, was shortlived. It finished in last place in its only season 1977, and was demoted back to the Victorian Leagues, but not to the Victorian State League, which it had been a member of from 1974-76, but to the equivalent of a third division. As part of the requirements for all Victorian NSL clubs in 1977, they had to field a reserve side in the senior Victorian second division. Mooroolbark finished in a relegation spot and upon their return to Victorian competition the Victorian Soccer Federation saw fit that Mooroolbark should commence 1978 in the Victorian Metropolitan League Division 3 (todays State League 3) as that is where their state league team would play.

Three relegations in four years saw the club sink to the Provisional Leagues, but steady progress through the 1980s saw the club re-enter the Victorian State League in 1990 for a two season stay, before gradually slipping down the divisions once more into Provisional League 1 South-East. A three-year tenure in the lower-ebbs of competition saw promotion to State League Division 3 South-East where they narrowly missed out on promotion by one point in 2005. As of 2008, Mooroolbark are playing in the Provisional League 1 South-East.