Based on the basic theory of molecular recognition , we design a organic molecules model to induce the crystallization of hydroxyapatite to synthesized tooth-like calcium phosphate/hydroxyapatite under a controllable way in vitro. The cross-linking of collagen on the dentin surface and extraneous collagen was optimized by varying the molar ratio of N,N-(3-dimethylaminopropyl)- N'-ethyl-carbodiimide hydrochloride (EDC) and N-hydroxysuccinimide (NHS) at a constant EDC concentration. CaCl2 and Na3PO4-12H2O solutions were added after the crosslinking process. X-ray photoelectron spectroscopic (XPS) and Fourier transform infrared spectroscopy (FTIR) analysis of organic protein monolayer for samples. The obtained composite were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM) as well as energy dispersive X-ray (EDX). XPS and FTIR analysis showed the surface organic compositions in experimental group is higher than that of normal dentin and decalcified dentin surface. The results showed that the dentinal tubule were blocked by neonatal hydroxyapatite layer which has a continuous structure of columns crystal with size of 10-40nm. Furthermore, there were column crystal with parallel direction inside, similar to the crystal array in the top of enamel rod. This study showed that the specific organic molecule model can be used as a potential effective crystal growth modifier.