The number of times its iOS apps were used reached 4.2 million in the last 12 months, up by 446,000 on the previous year.
Figures for Android devices show an increase from 855,600 to an estimated 966,000, bringing the predicted total across both operating systems to more than five million.
People spent an average of eight minutes on the Daily Prayer app, one of various digital platforms offered by the Church of England in a bid to attract more believers.
The trend comes as church attendances continue to fall across the UK, with the average weekly number of adults and children going to Sunday service declining by 15% from 2008 to 2018.
There were 1.12 million regular worshippers at Church of England churches in 2018, its latest statistics show.
However a church-finding website offers some hope, with a rise to 38 million page views in the last 12 months.
Last May, the Church of England launched its own Amazon Alexa skill for Amazon Echo smart speakers, which offers daily prayer resources to users and a church-finder capability.
Since releasing the service, the Alexa skill has been asked more than 100,000 questions by Christians and people exploring the faith.
“The digital figures show how people are using apps, smart speakers and social media to explore and engage in the Christian faith wherever they might be,” said Helen-Ann Hartley, the Bishop of Ripon.
“Christians have been praying the morning and evening offices for centuries and it is inspiring that this is available through new platforms and devices to meet the way people live now.
“The significant uplift in visits to AChurchNearYou.com is showing the interest people have in attending churches for weddings, christenings, funerals, services and when travelling.
“The Church’s digital innovation is enabling people to hear the good news of Jesus Christ in ways that weren’t previously possible alongside regular Sunday worship and at significant moments such as Christmas and Easter.”
The Church of England says social media engagement has increased from 2018, with an average reach of 3.6 million every month.