The singer, whose concert at the Manchester Arena was attacked by terrorists killing 22 people, was joined by a host of star names from the music world at the Emirates Emirates Old Trafford cricket ground.
Justin Bieber, Take That and Robbie Williams were just some of the popular acts who supported Grande to wow crowds.
Grande came out dressed in an oversized white One Love Manchester sweatshirt, ripped jeans and high-heeled black boots accompanied by a company of dancers wearing the same sweatshirts in black.
She performed her hits Be Alright and Break Free, shouting: “Manchester make some noise!” before pink streamers rained down on the crowd.
Concert-goers began queueing outside Lancashire Cricket Club’s Old Trafford ground from 8.30am ahead of the One Love Manchester gig.
Grande’s fans who were caught up in the Manchester bombing were offered free tickets for the event and said they were nervous to return to a concert so soon after recent terror attacks but determined to carry on to show solidarity with the victims.
Proceeds from the concert will go towards the We Love Manchester Emergency Fund, set up by Manchester City Council in partnership with the British Red Cross, to support grieving families and victims of the bombing.
A one-minute silence was held for the victims who lost their lives during the bombing at the concert last month.
Mumford and Sons frontman Marcus Mumford opened the concert, singing “you are not alone in this” as he performed an acoustic version of the band’s hit Timshel.
Mumford then welcomed Take That to the stage to open their set with their crowd-pleasing song Let It Shine.
In between renditions of Giants and Rule The World, Gary Barlow told the crowd: “Thank you everybody for coming out tonight, thank you for everybody watching at home, thanks to Ariana for inviting us tonight.
“Our thoughts are with everyone that’s been affected by this.
“We want to stand strong, look at the sky and sing loud and proud.”
Barlow welcomed former Take That bandmate Robbie Williams to the stage as “our friend, our brother,” before the foursome took a bow together and Williams led the crowd in a sing-along to his hit Strong, with the lyrics changed to ‘Manchester, we’re strong, we’re strong, we’re strong, we’re still singing our songs.”
Williams, who appeared to be wearing a sweatshirt from Justin Bieber’s Purpose world tour, then treated the audience to his anthem Angels.
U2 frontman Bono sent a video message to the concert, telling the crowds: “All our hearts are with you, all our hearts are with Manchester and with the UK.
“So many of our friends are in this great city.
“We’re broken-hearted for parents who’ve lost their children and children who’ve lost their parents in this senseless, senseless horror.
“There is no end to grief and that’s how we know there is no end to life.”
Pharrell Williams then opened his performance with a rendition of Get Lucky, his hit with Daft Punk, before Miley Cyrus joined him on stage to perform Williams’ hit Happy.
Before welcoming Cyrus to perform Happy, Williams said: “You know why I’m bowing, I’m bowing because despite all the things that have been going on in this place, I don’t feel or hear or see any fear in this building.
“All we feel here tonight is love, resilience and positivity and you know what, I hate to be corny, but it makes me ... “
After Williams left the stage Cyrus performed her song Inspired, after telling the crowd: “Manchester I just had to take a second to look around at all of you. I’d like to wrap my arms around each and every one of you and tell you thank you from the bottom of our hearts for having us.
“I’m so honoured to be at this incredible event surrounded by all you amazing people.
“The most important responsibility we have on this entire planet is to take care of one another.”
She continued: “I’ve always loved Manchester and not just tonight, it’s always felt like a home away from home to me.”
One Direction star Niall Horan performed his hit Slow Hands before dedicating song This Town to Manchester, saying: “I just want to say I’ve been lucky enough to travel all over the world and every time I come back to Manchester I’m addicted to this place.
“When I seen you guys all rallying together last week it was a sight to behold, it was incredible.
“We love you, we’re with you.”