Grande auditioned for the Nickelodeon television show Victorious in New York along with 13 co-star Elizabeth Gillies in 2009. In this sitcom set in a performing arts high school, Grande was cast as Cat Valentine. Grande had to dye her hair red every other week for the role because the executive producer, Dan Schneider, did not want all cast members to be brunettes, and the red hair was also a feature that the network felt would fit the personality of Cat.

Grande recorded her debut album, Yours Truly, over a three-year period. She completed the album, originally titled Daydreamin, in June 2013; it was released on August 30, 2013.She is credited as a songwriter on several tracks of the album.

By January 2014, Grande had begun recording her second studio album, with singer-songwriter Ryan Tedder and record producers Benny Blanco and Max Martin Grande is also credited as a songwriter on several tracks of the album.

In early 2015, Grande embarked on her extensive The Honeymoon Tour of North America and Europe, with a few stops in Asia.Following the tour's early commercial success, 40 more dates were added through October 15, 2015.Reviews of the tour performances have praised Grande's vocals and ability to convey emotion in the songs but found the concerts to be over-produced: "some judicious editing would've elevated the evening from surprising to satisfying and possibly even shockingly good. As it is, Grande is so busy piling on the spectacle she neglects to highlight the one thing – those deceptively powerful pipes – setting her apart from her contemporaries.The tour earned $14 million in its first 25 performances, selling 290,699 tickets.

Grande is scheduled to appear as Chanel #2, a recurring character, on the new Fox comedy-horror TV series Scream Queens, created by Ryan Murphy, starring Emma Roberts, Jamie Lee Curtis and Lea Michele.[103][104] Grande is also scheduled to launch her first fragrance, Ari, in September 2015.[105][106] She is set to appear in the upcoming comedy film Zoolander 2, starring Ben Stiller and Owen Wilson,and the upcoming TV reality show Knock Knock Live hosted byRyan Seacrest.

On May 29, 2015, Grande began to reveal lyrics of the "Intro" song of her new album on Twitter.Soon afterwards, Grande confirmed that her third studio album will be titled Moonlight.She revealed that she wrote the title track with Victoria Monet. She has also signed a publishing deal with Universal Music Publishing Group.