In 1800 Edward Bouverie Pusey was born at Pusey House. By his early twenties he was a learned and God-fearing man, and very fond of riding. His rides often took him through the hamlet of Littleworth, which did not have a church of its own and was considered a dire and lawless place. Those who might want to attend church had to walk across the fields to Faringdon church and when there was death in the village the coffin was carried along the same footpath. 

In 1823 Edward was elected a Fellow of Oriel College in Oxford. His first action was to propose the building of a church in Littleworth. He was helped by Rev. Page Eden, who persuaded Oriel College to give £500 to build a church and endow a new parish. At eleven o'clock on Wednesday 29 May 1839 the new church was consecrated as "The Church of the Holy Ascension".

At first the Vicar of Buckland was responsible for the church in Littleworth. By 1876 Littleworth had its own Vicar and the Vicarage was built in 1884 on land donated by Oriel College. There was a Vicar at Littleworth until 1971 when the Archdeacon arranged for a plurality for the three parishes of Littleworth, Buckland and Pusey. In 2002 it was agreed that Littleworth would become part of the Benefice of Churbury with Gainfield, a group of seven churches in rural Oxfordshire.