Wearing a sweat shirt graffitied with the legend One Love Manchester, Grande showed up several times throughout the three-hour show alongside Coldplay, Black Eyed Peas and Little Mix to celebrate the fighting spirit of Manchester.
"Manchester we're strong. we're still singing our song", he sang with the audience of 50,000.
Apart from that, the singer also belted out her hits "Break Free", "Side to Side", "Be Alright" and "The Way" with her boyfriend Mac Miller.
Sunday's concert will raise money for victims of the attack that struck at Grande's show on May 22.
Earlier this week the former Oasis frontman held a special gig in the city with all proceeds going to the We Love Manchester fund for victims and their families.
British singer Marcus Mumford held a moment of silence before opening the benefit concert.
Fans have praised pop star Ariana Grande after last night's emotional One Love Manchester benefit concert. The attack killed 22 and wounded dozens.
It included performances from Justin Bieber, Miley Cyrus, Liam Gallagher, Katy Perry, Coldplay and Imogen Heap, whose rendition of her cult meme classic 'Hide and Seek' went largely underreported.
On top of this, 1,078,000 requests were made on iPlayer making it the most popular live non-sports broadcast in its history. The baby then tried to sing along with the pop star herself. The event was arranged as a tribute to the victims of the Manchester Arena attack.
"First show back tonight".
Linda Tipping and Laura Mayren, from Chorley in northwest England, say they were determined to enjoy themselves even as London was reeling. "And I think if we can be this team until we're old, continue to do things like this, let's not stop today", Cyrus told the interviewer.
Ariana Grande paid tribute to the city of Manchester, England, on Sunday with an energetic, all-star concert that raised millions for victims of a suicide bombing that tore through her last performance in the city almost two weeks ago.