Grande had already re-released her 2014 hit "One Last Time" as a charity single, and her "One Love Manchester" concert album, available on Apple, Spotify and Tidal, is raising funds for the Red Cross charity as well.
Throughout the show, Grande became teary-eyed, expressing her gratitude to her Manchester fans.
Sunday's concert will raise money for victims of a suicide bombing that struck at the end of singer Ariana Grande's Manchester show May 22.
"From the moment the idea [of the benefit concert] came, I was very obsessed with it.[but] I had to slow my mind down because Ariana. didn't know if she could ever go on stage again".
'All week you have been incredible and as a friend, I'm so proud of you my love.
"I want to thank you from the bottom of my heart for being here today", the singer said between songs.
Following the gig, Ariana's One Last Time, which was first released back in 2015 as part of her My Everything album, looks set for number one this week. There is nothing I or anyone can do to take away the pain you are feeling or to make this better.