The College was opened in 1868, partly in response to the growth of the city. Secondary education under WM auspices had been available in Dublin since the 1840s. Sir William M'Arthur was prominent among the early benefactors. Composed of both a 'college' and a 'school', it aimed from the outset at providing education for boys from the earliest stages of schooling to the completion of a degree or entry into business life. Within months of opening it was agreed that 'young ladies' be admitted on equal terms. The school had places for day pupils and boarders and for the children of Methodist ministers. The college was for candidates for the ministry (transferred in 1919 to Edgehill College) and for lay undergraduates at the nearby Queen's College (later Queen's University). William Arthur was appointed its first Principal. In 1999 Methodist College had almost 1,900 pupils, including nearly 200 boarders and 500 in the preparatory departments.
An exceptionally strong musical tradition has achieved an impressive number of awards, including the UTV Grammar School Choir of the Year (by the girls' choir in 1996, 1998 and 2002) and the Radio 3 Choir of the Year, Children's Section (by the junior choir in 2005). The chapel choir has sung for a week in Westminster Abbey during the Abbey choir's summer vacation.