Based on the molecular recognition theory, an organic molecules model was designed to induce the hydroxyapatite crystallization, to build a tooth-like calcium phosphate/hydroxyapatite under a controllable way in vitro. The cross-linking of collagen on the dentin surface and gelatin 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. The whole process requires repeating the crosslinking and mineralization process for five times. The obtained composite were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM) as well as energy dispersive X-ray photoelectron spectroscopy (XPS). 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 was 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.