Whilst a councillor, he also served as an Associate Cabinet Member for Leisure, Culture, Localism and Young People.

[8] At the 2005 general election, Charalambous stood as the Labour Party candidate in Epping Forest, coming second with 21% of the vote behind the incumbent Conservative MP Eleanor Laing.

[9] Charalambous stood in Enfield Southgate at the 2010 general election, coming second with 32.2% of the vote behind the incumbent Conservative MP David Burrowes.

[20] At the 2019 general election, Charalambous was re-elected as MP for Enfield Southgate with a decreased vote share of 48.5% and an increased majority of 4,450.

[23] Charalambous swapped roles with Holly Lynch in a minor reshuffle in May 2021, becoming the Shadow Minister for Immigration.

[25][26] After a thorough investigation involving scrutiny by a board chaired by an independent lawyer, the complaint was not upheld and he had the whip restored in April 2024.