To develop a new kind of natural self-hardening bone-rehabilitative composite and to study the chemical and biomechanical properties and the biocompatibility of the natural self-hardening composite. The self-hardening composite was prepared by combination the natural hydroxyapatite (NHA) obtained from pig bones, chitosan, CaO and ZnO. The setting time, the exothermic temperature and the pH value of the self-hardening composite were performed during and after the hardening of the samples. Compressive strength of composite was measured 48h after the setting by using a universal testing machine and the microstructure of them was observed by using a SEM. Biological evaluations both in vitro and in vivo were also taken out. The setting time of self-hardening composite was 11.2