"The last time I hosted was in 2016, and we were right on the verge of electing our first female president," the 31-year-old singer and actor said in her monologue.
"So, I guess, second time's the charm?"
Grande, who first hosted in 2014, was doing it for the first time without also serving as a musical guest - a role that fell to Stevie Nicks - and promised not to sing, before breaking into a song.
Family Feud: Election Edition — Saturday Night Live - SNL (@nbcsnl) pic.twitter.com/x03aYhHKTXOctober 13, 2024
The theme continued as she vowed during the tune not to do her signature impressions of Britney Spears, Miley Cyrus and Gwen Stefani, before throwing out a bit of each.
She would do a much longer version of Celine Dion in a sketch later in the show.
Grande hosted to promote her movie musical Wicked, the Wizard of Oz prequel set to be released in November.
She said playing the good witch Glinda in the film was the dream of every theatre kid like her, after "losing their virginity".
Grande's episode comes amid a ratings spike for the sketch institution, likely brought on by its 50th season, and election season.
September's season premiere brought in the most viewers since 2020.
Just as in the first two episodes of the new season, Maya Rudolph played Vice President Kamala Harris in the night's cold open, leading a group of former cast members returning as guest stars including Andy Samberg as Harris' husband Doug Emhoff and Dana Carvey as President Joe Biden.
They teamed up for an election edition of The Family Feud, taking on team Trump.
Musical guest Nicks - appearing on the show for the first time in more than 40 years - opened with her new single The Lighthouse before performing Edge of Seventeen from 1981.
Michael Keaton will host the next episode, joined by musical guest Billie Eilish.
The onset of season 50 has brought reflection and nostalgia in many forms, including Saturday Night - a movie comedy dramatising the minutes before the first episode of the Lorne Michaels-helmed sketch institution on October 11, 1975.