Villongco's singing career began when she was only nine years old, prodded by her grandmother, showbiz industry crusader and former Movie and Television Review and Classification Board (MTRCB) chief Armida Siguion-Reyna.

She first gained public attention when she sang the theme song for the ABS-CBN children's television series Hiraya Manawari which was composed by Ryan Cayabyab.

Villongco then returned to theater, appearing in such roles as Hodel in Fiddler on the Roof and Ophelia in Ana Abad Santos-Bitong's steampunk-influenced Hamlet, for Repertory Philippines.

[2] In November 2016, she starred as Alison Bechdel in the first international production of Fun Home, which premiered in Manila, alongside Lea Salonga as Helen and Eric Kunze as Bruce.

Her solo 'Telephone Wire', about the pall of what's unsaid between Alison and her father during [an] ill-fated drive dramatically captured the inner turmoil that Villongco lugs with her even after the curtain call.