The effect of press process on the mechanical properties of PLLA and HA/PLLA was investigated. Bending modulus and bending strength were effectively improved by press process. The improvement was more effective in the uniaxial press than in the biaxial press due to higher level of molecular orientation. Mode I fracture energy was evaluated for the materials. FE-SEM observation of the fracture surfaces was also performed to characterize the effects of press process on microscopic deformation and failure behavior. Mode I fracture energy was dramatically improved due to the press process. The primary mechanisms of the improvement are thought to be crevasse-like failure at the interlayers of the layered structure created by press process and improved adhesion between HA particles and PLLA matrix.