The service featured an address, prayers and songs from the choir of Merton College, Oxford.
It marks closening ties between the Anglican and Catholic churches and is one of several examples of ecumenism between them in the last year.
In the last month Pope Francis became the first pontiff to visit an Anglican church in Rome.
And the Archbishop of Canterbury Justin Welby celebrated evening prayers with the pontiff in October last year.
While the relationship between the two churches is strengthening with an aim to eventually becoming one church, significant theological differences remain, for example the role of women in church leadership and ministry and the marital status of clergy.
Speaking on Premier's News Hour Archbishop David Moxon, the Archbishop of Canterbury's Representative to the Vatican, said: "We were delighted with the hospitality and care of the Vatican and of the archpriest of the Basilica who made us very welcome indeed.
"It was an historic moment really as we got closer together in prayer and song.
"The urgency of us acting together, praying together, is increasing as you look at the needs and wounds of the world. Basically God is saying to us: 'let's get our act together'.
Listen to Premier's Aaron James speaking to Archbishop David Moxon on the News Hour: