AbstractLight modulation is of paramount importance for photonics and optoelectronics. Here we report all-optical coherent modulation of third-harmonic generation (THG) with chiral light via the symmetry enabled polarization selectivity. The concept is experimentally validated in monolayer materials (MoS₂) with modulation depth approaching ~100%, ultra-fast modulation speed (<~130 fs), and wavelength-independence features. Moreover, the power and polarization of the incident optical beams can be used to tune the output chirality and modulation performance. Major performance of our demonstration reaches the fundamental limits of optical modulation: near-unity modulation depth, instantaneous speed (ultra-fast coherent interaction), compact footprint (atomic thickness), and unlimited operation bandwidth, which hold an ideal optical modulation solution for emerging and future nonlinear optical applications (e.g., interconnection, imaging, computing, and quantum technologies).