Natural bone is a kind of nanocomposites composed of orientated hydroxyapatite (HAp) along c-axis and fibrous collagen. Therefore, composites exhibiting composition and structure analogous to those of natural bone have been expected to be useful bone substitute materials. Organic polymer-HAp composites have been attracted much attention since they have interesting features such as bone-bonding ability, i.e. bioactivity and flexibility. In the present study, chitosan-HAp nanocomposites were prepared through mechanochemical reaction using conventional ball mill and subsequent aging. The obtained composites contained carbonate-containing HAp, and HAp nanocrystals in the composites aged at 25°C for 24 h showed a needle-like structure. They can form bone-like HAp on their surfaces after soaking in simulated body fluid (SBF), indicating potential for bioactivity in living body. The prepared chitosan-HAp composites are expected to be one of the useful bone substitute materials.