The current building of the Assumption Cathedral was constructed in 1848-1849 according to the design of Lewis Vulliamy and originally served as the Anglican parish church of All Saints. It replicates the architecture of the Basilica of San Zeno Maggiore in Verona, built in the 11th century. In 1892, the western facade was reconstructed by Harrison Townsend. Special attention is drawn to the painting above the high arches, created by Heywood Sumner in the technique of sgraffito, where the lower layers of different colors are revealed by scratching the upper layer of plaster. Above the eastern arch is depicted the Crucifixion with symbols of the evangelists, while in the western part, six round images symbolize the six days of Creation. The frescoes on the upper part of the nave walls represent biblical scenes and saints.

In 1956, the church was leased to the Orthodox community of the Russian Orthodox Church, which has existed since 1741. With the support of parishioners, the building was purchased in 1979. The complex also includes five residential buildings.

The building was easily adapted for Orthodox worship. The royal gates of the iconostasis were saved from the church at the Russian Embassy in London after the October Revolution. The icons of the iconostasis were created by three students of the famous Russian icon painter Leonid Uspensky at different times, and many other icons were donated by private individuals.

In 2006, Bishop Basil (Osborn), the temporary head of the Surazh Diocese, to which the cathedral belongs, decided to transition from the Moscow Patriarchate to the Constantinople Patriarchate. The Church of Constantinople accepted him, granting him the title "Amphipolis" and appointing him as vicar of the head of the Western European Exarchate.

In 2007, part of the clergy and laity of the Assumption Cathedral decided to follow Bishop Basil, declaring that the church in central London belonged to them. This led to a two-year court case that ended in favor of the Russian Orthodox Church. Those who left with Bishop Basil moved to St. Peter's Church in London.

In January 2014, renovations began at the cathedral, which had been needed since the lifetime of Metropolitan Anthony. During the work, services were held in a specially arranged room. The church reopened on December 31 of the same year. The parish community now includes people of various national backgrounds, primarily Russians and Britons, so services are conducted in Church Slavonic and English.