The church was designed by architect Frederick Walters and built by W. T. Morgan. The foundation stone of the church was laid on 20 January 1907 by Bishop Hedley and later that year, on 30 October, the altar was consecrated before the church opened on 3 December.[3] The tower was added in 1916.[1] The church is built using roughly dressed Pennant sandstone and cut Bath stone ashlar dressings, in a late 12th-century French style.[1]
In January 1941, the sacristies and St Ann's Chapel in the church were destroyed by an air raid to be rebuilt 10 years later.[3]
In 1952, the church was temporarily closed to repaint and clean the church as well as to install new lighting and amplifiers. The church was repainted again in 1962.[3]
It became a listed building in 1975, as a building of quality by a noted ecclesiastical architect.[1]
In 1991 the church came under the care of the Archdiocese of Cardiff after many years under the Benedictine community.
In January 2023, Archbishop Mark O'Toole appointed Rev. Canon David Hayman, the Chancellor of the Archdiocese of Cardiff, and parish priest of Pontypool, as the new parish priest.
The church underwent an internal reordering in 2000.[3]
The parish has taken responsibility for the parish records of Sacred Heart, Leckwith, Cardiff.[citation needed]
The babies of Charlotte Church and Gavin Henson were baptised at St Mary of the Angels church. Ruby Henson was baptised on 28 June 2008 by Fr. Delaney OSB, who Church described as her favourite priest.[6] Their son Dexter Lloyd Henson was christened in August 2009.[7]
In Charlotte Church's Confessional Song, one line is "Poor old Father Delaney", referring to the St Mary's parish priest.[citation needed]