Nanohydroxyapatite (HAP) was crystallized in an aqueous solution of carboxymethyl cellulose (CMC) to prepare the composites of CMC and HAP with a stable interface between them with the aim of developing a sustainable tough biomass composite material inspired by bone. The temperature (room temperature to 90 °C) and the concentration of CMC (0.83–13.2 g/L) were optimized for the mechanical properties of the composites. The composite containing 67 wt % HAP prepared at 50 °C in the presence of 9.9 g/L CMC exhibited the largest flexural strength of 113 ± 2 MPa and the elastic modulus of 7.7 ± 0.3 GPa. X-ray diffraction showed that nanometer-sized HAP crystals were formed with a large aspect ratio, and energy-dispersive X-ray spectroscopy and infrared spectroscopy revealed that CMC was bound to the surface of HAP through an ionic interaction between Ca 2+ and COO – . Since the composite has a higher flexural strength than polyamide 6 (92 MPa) and a higher elastic modulus than polyamide 6 with 40 wt % glass fiber (5.5 GPa), it can be used as new tough biomass composite material to replace petroleum-derived engineering plastics.