The singer told Metro that the group are currently collaborating with the 'Grenade' star.
Asked about his dream hook-ups, Merrygold said: "We're working with Bruno Mars at the moment and I've admired his work for ages.
"Then maybe Usher or Rihanna. We're in talks and it would be amazing if it happened."
Meanwhile, Merrygold brushed aside suggestions that he, Marvin Humes, Jonathan 'JB' Gill or Oritsé Williams would ever quit the band for a solo career.
Quizzed on who would be first to leave the group, he said: "No-one. If JLS ever does end - which it won't - it'll be all four of us. We'll be friends forever. The group works and we're happy as we are."