The American singer appeared in front of an estimated 50,000 fans at the One Love Manchester show less than two weeks since her gig was targeted by a suicide bomber.
Grande had arranged Sunday's concert at Manchester's Old Trafford cricket ground in tribute to the 22 people killed and 116 injured at the Manchester Arena on 22 May.
The 23-year-old star arrived on stage an hour into the show, for which there were extra security measures in place following Saturday night's terror attack in London.
Grande wore a white jumper emblazoned with the slogan One Love Manchester as she performed.
Many in the crowd were in tears as Grande sang with a choir from Parrs Wood High School, who have raised thousands of pounds for the families of the bombing victims.
Grande comforted soloist Natasha Seth, who was overcome with emotion, mouthing to the schoolgirl: "Babe, it's ok."
Some members of the choir had been present at the tragic 22 May show.
Grande asked the crowd: "Tonight is all about love, am I right?"
She added: "I want to thank you all from the bottom of my heart for coming today, I love you so, so much. Thank you.
"I think the kind of love you're displaying is the kind of medicine the world really needs right now. So I want to thank you for being just that."
Grande described how she changed her plans for the show after the mother of bombing victim Olivia Campbell had revealed the 15-year-old "would have wanted to hear the hits".
She joined Coldplay to perform Oasis hit Don't Look Back In Anger, to recall how city centre crowds had spontaneously burst into a rendition of the song in the days after the Manchester bombing.
All of those who had attended Grande's concert last month had been offered free tickets to Sunday's show, while those who were still recovering from their injuries in hospital were watching on TV.
The large crowd had fallen at the start of the concert to remember those who were killed and injured in both Manchester and London.
Kicking off the concert, Marcus Mumford told concert-goers: "Let's not be afraid."
His performance was followed by Take That, with star Gary Barlow telling the crowd: "Our thoughts are with everyone that's been affected by this but right now we want to stand strong, look at the sky, sing loud and proud."
Robbie Williams then led the thousands inside the venue in a chorus of: "Manchester, we're strong, we're strong, we're strong.
"We're still singing our songs, our songs, our songs."
Image:The crowd at Old Trafford for the One Love Manchester concertDuring a rendition of his hit song Angels, Williams told the crowd: "I need you on this one."
Describing the "emotional" atmosphere at Old Trafford, Sky's Entertainment Correspondent Katie Spencer said: "It's turning into a real celebration of community spirit and people coming together.
"Everyone's joining in, everyone wants to sing out with one voice."
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