Three types of calcium phosphate porous materials were prepared by the applied hydrothermal method. One of them was non-stoichiometric hydroxyapatite (HA) with calcium deficient composition and the others were β-tricalcium phosphate (β-TCP) and HA/β-TCP bi-phase material. Granules with several millimeter in size of calcium deficient HA, β-TCP and HA/β-TCP could be prepared. These granules with porosity over 70 % were composed of rod-shaped particles with aspect ratio about 10. Rod-shaped particles were locked together to make sub-micro-sized pores of about 0.1 to 0.5 µm in size. These materials must be suitable for the bone graft materials and as the scaffolds of cultured bone.