Two-dimensional molybdenum borides (MBenes) comprise a new class of 2D transition metal borides that exhibit potential photonics applications. Recently, the synthesis of individual single-layer MoBT (T = O, F, OH) MBene sheets has been realized, which attracted considerable attention in optoelectronics. However, there is still a lack of understanding and regulation of the photophysical processes of MoBT MBene. Here, we demonstrate that MoBT MBene exhibits a surface termination-dependent electronic structure, carrier dynamics, and nonlinear optical response over a wide wavelength range (500-1550 nm). As prepared 2D MoBF MBene possesses a semimetal material property that exhibits a shorter intraband scattering process (<100 ps) and a considerable nonlinear optical response at a broadband cover optical communication C band at 1550 nm. These thrilling results are confirmed theoretically and experimentally. The analysis of these results adds to the regulating and understanding of the basic photophysical processes, which is anticipated to be beneficial for the further design of MBene-based photonics and nanoelectronics devices.