Bulk metallic glass (BMG) has received consistent attention from the research community owing to its superior physical and mechanical properties. Modulating and controlling the surface functionalities of BMG can be more interesting for the surface engineering community and will render more practical applications. In this work, a facile laser-based surface texturing technique is presented to modulate and control the surface functionalities (i.e., wettability and hardness) of Zr-based BMG. Laser surface texturing was first utilized to create periodic surface structures, and heat treatment was subsequently employed to control the surface chemistry. The experimental results indicate that the laser textured BMG surface became superhydrophilic immediately upon laser texturing, and it turned superhydrophobic after heat treatment. Through surface morphology and chemistry analyses, it was confirmed that the wettability transition could be ascribed to the combined effects of laser-induced periodic surface structure and controllable surface chemistry. In the meantime, the microhardness of the BMG surface has been remarkably increased as a result of laser surface texturing. The facile laser-based technique developed in this work has shown its effectiveness in modification and control of the surface functionalities for BMG, and it is expected to endow more useful applications.