The proposal to establish a Unitarian place of worship in Croydon was first made at a meeting of six gentlemen held on 20 May 1870 at the house of Maurice Grant. As a result, a congregation was formed under the title of Croydon Free Christian Church: the word Unitarian was deliberately avoided in order to avoid any suggestion of doctrinal allegiance. RR Suffield was appointed as Minister, and gave his first address on 2 October: he continued to serve until his resignation through ill health in 1877. The government of the church was placed in the hands of a General Purposes Committee, soon known simply as the Committee. Other committees included a Trust Deed Committee, a Finance Committee, and a Music Committee.
The congregation bought the Iron Church (formerly a Baptist Church) in Wellesley Road. It was opened as the Free Christian Church on 11 December 1870. The freehold of the land was bought in 1875. Subsequently, a new, permanent, church was built on the same site: the memorial stone was laid on 20 April 1883, and it was formerly opened on 17 November 1883. The Iron Church had been moved to the rear of the new building: it was renamed the Social Room, and was put to regular use for soirees, dances, childrens parties, etc.
The Church attracted a relatively small, educated, middle class congregation, and its early ministers included several capable intellectuals. However, relations between minister and congregation were sometimes turbulent. EM Geldart, after some years as a popular minister, antagonised many of his congregation when he began to preach a doctrine of Social Democracy: the strain affected his health, and he died in mysterious circumstances soon afterwards. His successor, CJ Street, resigned over differences of opinion with the congregation; WM Weston was criticised for some of his views (notably an address advocating the abolition of the traditional home), and resigned to rejoin the Roman Catholic Church; and WW Chynoweth Pope was asked to resign following a difficult period of declining attendances. Only after the appointment of GC Sharpe in 1921 did relations become more consistently harmonious.
Among the prominent early members of the congregation were Henry Moore and his family. In 1906 his son, H Keatley Moore, paid an official visit during his term of office as Mayor
The Church was badly damaged during World War 2; and, as a result, a new Church and hall were built in Friends Road in 1958. In 1960 the Church was renamed the Unitarian and Free Christian Church.