The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here, we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observed optical damping and antidamping of mechanical vibrations as well as the optical spring effect. The exciton-optomechanical coupling strength is also gate-tunable. Our observations can be understood in a model based on photothermal backaction and gate-induced mirror symmetry breaking in the device structure. The observation of gate-tunable exciton-optomechanical coupling in a monolayer semiconductor may find applications in nanoelectromechanical systems (NEMS) and in exciton-optomechanics. © 2021 American Chemical Society. All rights reserved.