To investigate the grinding removal mechanism of multispectral CVD zinc sulfide which is widely used in manufacturing infrared optical component, microscopic indentation and diamond single scratching experiment were carried out on polishing surface of zinc sulfide, and zinc sulfide was ground by diamond wheel. The elastic and plastic deformation were found in mechanical removal process of zinc sulfide. Crack and fracture were extended along the grain boundary, scratching direction, and grinding marks direction. And, crack initiation and propagation could be suppressed with lower press, lower crack and fracture would be obtained by cuspidal diamond abrasive. Besides, periodic and scattered grinding marks were found from center to edge by cross grinding. This work provides references and ideas for ultra-precision grinding aspheric lens of multi-spectral CVD zinc sulfide.