Polycrystalline ZnS is a typical infrared optical material. It is widely used in advanced optical systems due to its excellent optical properties. The machining accuracy of polycrystalline ZnS optical elements must satisfy the requirements of high-performance system development. However, the soft and brittle nature of the material poses a challenge for high-quality and efficient machining. In recent years, in situ laser-assisted diamond cutting has been proven to be an effective method for ultra-precision cutting of brittle materials. In this study, the mechanism of in situ laser-assisted cutting on ultra-precision cutting machinability enhancement of ZnS was investigated. Firstly, the physical properties of ZnS were characterized by high-temperature nanoindentation experiments. The result revealed an increase in ductile machinability of ZnS due to plastic deformation and a decrease in microhardness and Young's modulus at high temperatures. It provided a fundamental theory for the ductile-brittle transition of ZnS. Subsequently, a series of diamond-cutting experiments were carried out to study the removal mechanism of ZnS during in situ laser-assisted cutting. It was found that the mass damage initiation depth groove generated by in situ laser-assisted cutting increased by 57.99% compared to the groove generated by ordinary cutting. It was found that micron-sized pits were suppressed under in situ laser-assisted cutting. The main damage form of HIP-ZnS was changed from flake spalling and pits to radial cleavage cracks. Additionally, the laser can suppress the removal mode difference of different grain crystallographic and ensure the ductile region processing. Finally, planning cutting experiments were carried out to verify that a smooth and uniform surface with Sa of 3.607 nm was achieved at a laser power of 20 W, which was 73.58% better than normal cutting. The main components of roughness were grain boundary steps and submicron pit. This study provides a promising method for ultra-precision cutting of ZnS.