Functional inorganic ZnO nanoparticles (ZnO NPs) have been designed and prepared, used as UV photosensitizers and reinforcing agents applied to waterborne polyurethane acrylate (WPUA) composite coating. The ZnO NPs are modified by the silane coupling agent, and the WPUA@ZnO NP composite coatings photoinitiated with different ZnO NP contents are prepared, their structure and properties are characterized by FTIR, XRD, SEM, BET, TG, and pencil hardness tester. The UV absorption of the inorganic photosensitizer ZnO NPs and the organic photosensitizer 1-hydroxycyclohexyl phenone (184) in the composite coating is tested and analyzed separately by DRS UV-3600 spectrophotometer. Three fabric-based materials (cotton, PET, and PP) are dipped into the WPUA@184 composite emulsions and WPUA@ZnO NP composite emulsions, and their mechanical properties, water absorption and water contact angle (WCA) are tested. The results show that the absorbance of the WPUA@ZnO NP composite coating is 40.28% higher than that of the WPUA@184 composite coating. Compared with the PP-WPUA@184 coatings, the stress of the PP-WPUA@ZnO NP coatings increases by 41.19% and the strain increases by 34.39%. The water absorption of the cotton and PET coatings decreases under the three conditions. Their hydrophilicity and hydrophobicity are changed, and the fabric-based coatings can be tuned for interfacial properties.