A mild and facile strategy to coat natural rubber (NR) with a hydrophilic coating is described that uses light and photoinitiator copolymers. Five high molecular weight photoinitiator copolymers, composed of hydrophilic (e.g., 2-hydroxyethyl acrylate [HEA], poly(ethylene glycol) [PEG], N-vinylpyrrolidone [NVP], N-isopropylacrylamide [NIDAM], and acrylic acid [AA]) and hydrophobic benzophenone (BP) units, are synthesized and evaluated for coating NR on UV irradiation. When the HEA/BP, NVP/BP, and AA/BP macromolecular photoinitiators attach to the NR surface, the latter becomes hydrophilic. The resulting hydrophilic coatings on NR sheets are analyzed via FT-IR spectroscopy, scanning electron microscopy, atomic force microscopy, contact angle measurements, and transwell cytotoxicity assays using NIH 3T3 fibroblast cells. The addition of high molecular weight hydrophilic polymers (e.g., polyvinylpyrrolidone and poly(2-methacryloyloxyethyl phosphorylcholine)) to the coating further enhances the coating's hydrophilicity and lubricity. The application of these non-cytotoxic, hydrophilic, and lubricious coatings on NR expands current applications and usage of NR.