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Grace Congregational Church dates back to the fall of 1920, when a group of Congregationalist leaders came together at the request of the New York Congregational Conference to discuss the possibility of organizing a Congregational church in Harlem. In June 1921, the Rev. Alexander C. Garner was called from Plymouth Congregational Church in Washington, D.C., to accept the responsibility of gathering members, organizing them and developing a Congregational church. Early meetings with about 30 persons were held in the auditorium of the 137th Street YMCA. The fledgling group eventually merged with the Harlem Latter-day Congregational Church at 250 West 136th Street, and the combined congregations were known as The Grace Congregational Church of Harlem.

In 1923, the society purchased the former Swedish Immanuel Congregational Church, located at 310 West 139th Street. Designed by Joseph Ireland, this plain brick structure was built in 1892 for the Lenox Presbyterian Church, who remained there until 1905 when they moved to 141st Street and St. Nicholas Avenue.

Since its beginning, Grace Congregational Church has been noted for its ministry to actors and musicians. Today the congregational is affiliated with the United Church of Christ.