The generation process, influence of the laser parameters on the production of zinc metal (Zn⁰), and the mechanism of interaction between the laser and ZnS were studied. It was observed that an increase in the number of S defects enhanced the quantity of Zn²⁺ ejected from the ZnS crystals, which increased the possibility of Zn²⁺ bonding with electrons to produce Zn⁰. A maximum Zn⁰ content of 9.3% in the products was detected upon changing the laser parameters. Upon analyzing the changes in the surface topography during the laser interaction with ZnS, it was shown that the interaction mechanism between laser and ZnS had a synergistic effect comprised of photochemical and photothermal processes, in which the photochemical mechanism predominated.