Synthesis of hydroxyapatite (HAp) oriented arrays is difficult but significant in biomineralization research for biomaterials. Herein, a novel strategy for the synthesis of HAp nanorod/nanosheet oriented arrays has been developed in the presence of biomolecules of creatine phosphate (CP) using solvothermal treatment in mixed solvents of N,N-dimethylformamide (DMF) and water. In this reaction system, CP biomolecules act as an organic phosphorus source and a soft template for the formation of HAp oriented arrays. This method does not need any hard template or surfactant, avoiding the procedures and cost for their removal from the product. The products are characterized with X-ray powder diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy and thermogravimetric analysis. The formation mechanism of HAp nanorod/nanosheet oriented arrays is discussed.