The nanocomposites were prepared by synthesizing (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO)-oxidized cellulose nanofibrils (TCNFs) or cellulose nanocrystals (CNCs) with hydroxyapatite (HA) in varying composition ratios in situ. These nanocomposites were first obtained from eggshell-derived calcium and phosphate of ammonium dihydrogen orthophosphate as precursors at a stoichiometric Ca/P ratio of 1.67 with ultrasonication and compressed further by a uniaxial high-pressure technique. Different spectroscopic, microscopic, and thermogravimetric analyses were used to evaluate their structural, crystalline, and morphological properties, while their mechanical properties were assessed by an indentation method. The contents of TCNF and CNC were shown to render the formation of the HA crystallites and thus influenced strongly on the composite nanostructure and further on the mechanical properties. In this sense, the TCNF-based composites with relatively higher contents (30 and 40 wt %) of semicrystalline and flexible TCNFs resulted in smoother and more uniformly distributed HA particles with good interconnectivity, a hardness range of 550–640 MPa, a compression strength range of 110–180 MPa, an elastic modulus of ~5 GPa, and a fracture toughness value of ~6 MPa^1/2 in the range of that of cortical bone. Furthermore, all the composites did not induce cytotoxicity to human bone-derived osteoblast cells but rather improved their viability, making them promising for bone tissue regeneration in load-bearing applications.

Hydroxyapatite (HAp) has long been considered the gold standard in the biomedical field, considering its composition and close resemblance to human bone. However, the brittle nature of hydroxyapatite (HAp) biomaterial, constrained by its low fracture toughness (of up to 1.2 vs. 2–12 MPa m^1/2 of human bone), remains one of the significant factors impairing its use in bone regeneration. In the present study, HAp nanoparticles synthesized by the solid-state (SHAp) and sonochemical (EHAp) approaches using eggshell-derived calcium hydroxide and ammonium dihydrogen orthophosphate as precursors are compared with those synthesized using commercially available calcium hydroxide and ammonium dihydrogen orthophosphate as precursors (CHAp) employing sonochemical method. The HAp samples were then compressed into compact materials using a uniaxial high-pressure compression technique at a preoptimized load and subsequently characterized for mechanical properties using the Vickers indentation method and compressive strength testing. The analysis revealed that the material with smaller particle size (30–40 nm) and crystalline nature (EHAp and CHAp) resulted in mechanically robust materials (σ_m = 54.53 MPa and 47.72 MPa) with high elastic modulus (E = 4011.1 MPa and 2750.25 MPa) and density/hardness-dependent fracture toughness (σ_f = 4.34 MPa m^1/2and 6.57 MPa m^1/2) than SHAp (σ_m =28.40 MPa, E = 2116.75 MPa, σ_f = 5.39 MPa m^1/2). The CHAp material was found to be the most suitable for applications in bone regeneration.