This paper aims at increasing the forming accuracy of microgrooves by using electroless plated Nickel Phosphorus (Ni-P) as the mold material in glass molding press (GMP) process. The mechanical characteristics and the performance of amorphous Nickel Phosphorus (a-Ni-P) plating layer were experimentally tested. In order to bring down the deformation of the a-Ni-P mold and increase the forming accuracy of microgroove molding, polycrystalline Nickel Phosphorus (c-Ni-P) was developed by heat treatment. With the increase of the hardness after crystallization, the plating layer shape changes due to the heat treatment, and the strategy to deal with the deformation and the techniques to produce c-Ni-P mold are generalized. Finally, the performance of c-Ni-P mold was experimentally tested, which confirms that c-Ni-P is an excellent mold material for glass microgroove forming.