Hybrid nanoparticles composed of chitin nanowhiskers (ChNWs) and gold nanoclusters (AuNCs) having an improved stability were prepared. The grafting of monomethoxypoly(ethylene glycol) (mPEG) and subsequent surface adsorption of AuNCs enabled the steric stabilization of ChNW/AuNC hybrids. mPEGs with terminal formyl groups and diethylacetal protecting groups were grafted via in situ deprotection and reductive amination with the surface amino groups (SAGs) of ChNWs. The treatment of chitin with a 30% sodium hydroxide solution improved the SAG contents of the ChNWs obtained from acid hydrolysis, resulting in an enhancement in mPEG grafting. The obtained sterically stabilized ChNW/AuNC hybrids exhibited remarkable dispersion stability at higher AuNC and electrolyte concentrations.