There appears to have been a chapel here in 1535 but no trace of this now remains. Chittoe was a detached portion of Bishop's Cannings parish and marriages and burials took place in the parish church there. This necessitated a long return walk across Bromham and Heddington and into Bishop's Cannings. In the late 18th and early 19th centuries this changed and baptisms and burials took place at nearby Bromham church although marriages still had to take palce at Bishop's Cannings. Through the efforts of Archdeacon MacDonald, vicar of Bishop's Cannings, Mrs Charlotte Starky and Bishop Denison of Salisbury, the church of St. Mary was built in 1845. It is in the Decorated style with a nave and chancel and having 172 free seats. A vicarage was built on a hill overlooking the church in 1846.
In 1867 the recently created parish of Chittoe was enlarged to inlude Westbrook and Sandy Lane and in 1870 the church was enlarged and improved. A north transept was added to provide a family area for the Spicers of Spye Park while the organ that had previously blocked the chancel was moved to a chamber adjoining this transept. Haden's hot air heating system was installed and the cost of £740 for the new transept was paid by Major Spicer. Parishioners raised the money to renovate the rest of the church and lay coloured tiles on the floor. In 1878 there was subsidence at one end of the church and a plan to rebuild the church on higher ground was put forward. This was not followed up but the foundations were strengthened instead. The roof was renewed and the church redecorated in 1879. A dwindling population and congregation caused the church to close and it was converted into a private house in the 1980s. There is still access to the graveyard. The parish registers for christenings and marriages dating from 1846 are held in the Wiltshire and Swindon History Centre at Chippenham.