The outspoken journalist called out the singer two weeks ago after she flew back to the U.S. immediately after a suicide bomber detonated an explosive inside Manchester Arena, where Grande had just played a concert.
"Manchester, we're gonna be all right", she yelled.
The 23-year-old pop star, who had to leave Manchester after the horrific attack at her May 22 concert here, made sure that her return filled the entire city with joy and happiness once again.
"I don't want to feel or hear or see any fear in this building", USA singer Pharrell Williams told the crowd as he led them in a rendition of his hit single "Happy".
The event is expected to bring in upwards of $3 million, which will benefit the We Love Manchester Emergency Fund, set up by Manchester City Council in partnership with the British Red Cross.
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Grande also ushered in artists like Little Mix and Imogen Heap, while Stevie Wonder was featured in a video segment where, while strumming his keyboard declared, "Love is truly the key, I don't care what ethnicity you are, what religion you are. Thank you so much for your donations".
"No matter how many hit songs she had, and no matter how incredible her concerts were - and he was always the first one there, applauding, kissing her, being in the front row - after every show, he would say, 'Ariana you know what song you have to sing?"
Before Grande's appearance, the star's manager Scooter Braun told the crowd: "Last night, this nation was challenged and all of you were challenged and you had a decision to make if you were going to come out here tonight".
"Seeing you guys coming together was a sight to behold, we love you, we are with you, the whole world is watching", he told the crowd.
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"My heart, prayers and deepest condolences are with the victims of the Manchester Attack and their loved ones".
The concert also will be broadcast on more than 130 iHeartRadio stations, and MTV will livestream the event on the website www.onelovemanchester.mtv.com.
The show opened with a minute of silence for those killed and injured in the attack.
"We will not quit or operate in fear".
On Friday, Grande visited some of her injured fans at the Royal Manchester Children's Hospital.
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For example, Cain noted that one of their youth service librarians will be putting on a Solar Eclipse Party on August 21 at 2 p.m. Hallauer said kids would be able to play a variety of video games from different gaming systems, such as Game Cube and Xbox.