The singer and "Voice" coach took the stage to perform her new single "Malibu," but took a moment beforehand to acknowledge the incident that left at least 22 people dead and 59 people injured, including children and teens.
"I'd like to dedicate this song to my good friend Ariana Grande and everyone who experienced that horrific attack yesterday," Cyrus said. "Our hearts are with you."
Cyrus joins a chorus of other celebrities and performers who have shown their support in the aftermath of the attack that occurred following Grande's performance at Manchester Arena on Monday.
Katy Perry, Taylor Swift, Selena Gomez and Harry Styles have all offered their condolences.
Usher and "Voice" contestant Chris Blue also shared a moving duet of R.E.M.'s "Everybody Hurts" that host Carson Daly said was meant to "lift people up" in light of the events in Manchester.
Blue was crowned the winner of the season at the end of the two-hour finale.
On Tuesday, Grande was spotted arriving at her home in Florida, having flown there from the U.K.
Earlier in the day, a source told CNN the singer was suspending her "Dangerous Woman" tour, which was set to include upcoming concerts this week at London's O2 Arena.
Grande's label -- Republic Records -- and tour promoter AEG Live have not yet given official word on when it may resume, if at all.