This study investigated a simple and low‐cost method for synthesizing graphene nanosheet/chitosan (GNS/CS) composites. The method involved (1) exfoliating graphite to prepare graphite intercalation compounds (GICs) using environment‐friendly ultrasonic energy and intercalating techniques, (2) preparing a high‐concentration GNS/CS dispersion from a mixture of GICs and CS, and (3) producing GNS/CS composites with varying GNS levels by adding the GNS/CS dispersion to CS. By incorporating 0.6 wt% GNS into a CS matrix, the mechanical and electrochemical properties of the resultant GNS/CS composite were markedly improved. Maximum enhancements of 29% and 39% in the elastic modulus and hardness of CS, respectively, were obtained. Furthermore, GNS/CS redox peak currents increased sevenfold relative to a CS‐modified electrode. POLYM. COMPOS., 39:4217–4223, 2018. © 2017 Society of Plastics Engineers