Hydroxyapatite (HA) was widely used in tissue engineering, because of its excellent biocompatibility and biological activity. In this study, HA powder was modified using amorphous aluminosilicate (AAS). HA/AAS hybrids were synthesized via a wet precipitation method. Composites of HA–AAS/chitosan–gelatin polymer were prepared and characterized using X-ray diffractometry, Fourier-transform infrared spectroscopy, transmission electron microscopy, scanning electron microscopy, pore size distribution, and surface area measurements. The results show that HA with a rod-like structure and sheets of AAS were connected via a chitosan–gelatin network in the formation of the composites, leading to high reduction in their specific surface area due to polymer coating. Biocomposites with lower content of AAS nanoparticles exhibited a compressive strength in the range of 3.1 to 7.3MPa and Young's modulus in the range of 0.11 to 0.21GPa, which were located within the range of human cancellous bone that have the range of 2–12 MPa and 0.05–0.5GPa, respectively. The bioactivity study proved that the composites samples enhance proliferation of preosteoblast cells (MC3T3-E1) and exhibit a lower toxicity than powder samples. Such findings shed light on HA-AAS/ chitosan–gelatin composites, as multifunctional materials for use in cancellous bone applications in the future.