Zinc and its alloys have garnered significant attention in the field of biological implantation due to their biodegradable, osteogenic, and mechanical properties. However, the degradation of zinc and its alloys always lead to an increase in local ion concentration, and the bare metal surfaces lack biocompatibility for implantation. To address these issues, a layer of calcium–phosphorus (CaP) coating was prepared on the surface of a Zn-0.5Li alloy. The micro-structure of the coating was observed with scanning electron microscopy (SEM) and a white light interferometry microscope. The phases of the coatings were characterized through X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The bonding strength between the coating and substrate was investigated using a scratch tester with a diamond stylus, and the corrosion properties were assessed using an electrochemical method. For the evaluation of biocompatibility and osteogenic properties, MC3T3-E1 cells were cultured on the coating. Live/dead staining and proliferation tests were performed to assess cell viability and growth. Cell adhesion morphology was observed with SEM, and the level of alkaline phosphatase (ALP) in the MC3T3-E1 cells cultured on the material surface was evaluated by ALP staining and activity measurement. The CaP coating on the zinc alloy surface improved the alloy’s biocompatibility and osteogenic property, and could be a promising surface modification option for a biodegradable zinc alloy.