The cosmetics industry is experiencing a rise in the demand for eco-friendly products due to growing environmental awareness. In response, eco-friendly forms of raw materials, production processes, and packaging have been developed. For hair products, the research focus is on a harmless method of crosslinking hair using eco-friendly raw materials. In this regard, we have recently proposed clean and nontoxic one-step protein crosslinking using eco-friendly chemicals composed of riboflavin phosphate (RFP), citric acid (CA), and polyols. In this study, we further explored the optimal concentration that induced maximum hair cross-linking by adjusting the ratio of CA, isopentyldiol (IPD), and sorbitol required for hair keratin protein cross-linking. Various combinations of CA in the range of 0.5−3% and IPD and sorbitol in the range of 1−5% were used to induce RFP-mediated photo-cross-linking. As a result, the combination of CA 3%, IPD 5%, and sorbitol 3% induced optimal cross-linking and increased tensile stress and Young's modulus of hair by 41% and 44%, respectively. In addition, RFP treatment was applied to black, brown, and blond hair to confirm the variation in the photo-cross-linking reaction according to hair color. Photo-cross-linking was successfully induced in the hair of all colors, and the increase in mechanical properties and hair-setting effect were verified. Hair color had no discernible impact on visible light-mediated cross-linking. Lastly, we demonstrated that the visible light-mediated cross-linking method we developed can be used for any hair color, and it is expected to be widely adopted as an environmentally friendly hair care product.