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Arbutin, a natural polyphenol, possessesnumerous biological activities including whitening, antioxidant,anti-cancer, anti-inflammatory activities, as wellas strong reducing power, making it an ideal bioactiveingredient for preparing gold nanoparticles (GNPs). Previously,we developed a novel green, mild syntheticmethod for GNPs using glycosides such as arbutin asreducing agents and stabilizers. Herein, we optimized thesynthetic method for glycoside–GNPs using arbutin,methyl b-D-glucoside, and phenyl b-D-glucoside and validatedtheir whitening efficacy in vitro and in vivo. Theresulting glycoside–GNPs were predominantly mono-dispersedand spherical (10.30–17.13 nm diameter). Comparedwith arbutin itself, arbutin–GNP complexes (GNPA1and GNP-P2) displayed enhanced whitening capabilities. Furthermore, GNP-P2 exhibited enhanced anti-inflammatoryactivity and lacked the toxicity associated witharbutin. Bioactive glycoside–GNP complexes may opennew directions for cosmeceuticals, and GNP-P2 may serveas a useful whitening ingredient in future cosmeceuticalapplications.