Hydroxyapatite is the well known bioactive ceramic used in medical and dental fields as blocks and particles, while chondroitin-sulfate is a dominant polysaccharide component of cartilage. Novel composite materials consisting of hydroxyapatite [Ca10(PO4)6(OH)2] and chondroitin-sulfate were synthesized by a coprecipitation method with a H3PO4 solution and a Ca(OH)2 suspension, one of which contain chondroitin-sulfate, and were consolidated under a cold isostatic pressure. The composites were evaluated by X-ray diffractometry, Fourier transformed infrared spectroscopy and transmission electron microscopy. In the composites, hydroxyapatite nanocrystals contained calcium-deficiency and a small amount of carbonate ions like human bone minerals and their c-axes were aligned along chondroitin-sulfate molecules by a self-assembly mechanism.