The van and knife attack on London Bridge and in Borough Market, which killed seven people, lead to nearby Southwark Cathedral being closed until further notice.
St Mark's Church in Kennington told Premier "there was no question" that they would agree to take over hosting the landmark's Pentecost service.
Rev Steve Coulson from St Mark's said: "It was a priviledge for us as a church to serve the Cathedral and to serve the wider diocese. It would have been really sad if the service had simply been cancelled and people hadn't come."
Les Isaac preaching this evening #ThyKingdomCome pic.twitter.com/g6q12wxQTI
— St Mark's Kennington (@stmarksken) June 4, 2017
More than 200 people attended the service at St Mark's, significantly more than the 30-40 who regularly attend their Sunday evening services.
Rev Coulson added: "About 150 candles were lit as people just came and made their own quiet prayers, reflecting on their own emotios and thoughts. At the same time, it was a real Pentecostal celebration of lively, noisy, cheerful music.
"There were a lot of clergy there actually who earlier in the day had been probably comforting and strengthening their own congregations and just helping their own churches through the emotions."
The Cathedral remains closed due to ongoing @metpoliceuk investigation. We will be posting updates when we receive them #LondonBridge
— SouthwarkCath Events (@Southwarkcathed) June 5, 2017
Responding on Sunday to the attack - which also saw three attackers shot dead by police - Very Rev Andrew Dunn, Dean of Southwark Cathedral appealed for prayers.
Click here to listen to Premier's Alex Williams speaking with Rev Steve Coulson: