This study reported a novel and facile method for the spontaneous synthesis of flowerlike cobalt phosphate nanocrystals (Co 3 (PO 4 ) 2 nanoflowers) without adding any templates, and the growth mechanism was further studied. Subsequently, an excellent nanobiocatalyst system was established via the biomimetic mineralization of cobalt phosphate with Co-type nitrile hydratase (NHase). Because of the interactions between Co ions in the microenvironment of cobalt phosphate and enzyme active site, the encapsulated NHase (NHase@Co 3 (PO 4 ) 2 ) exhibited high catalytic efficiencies and desirable stabilities. The enzymatic activity of encapsulated NHase was 238.4 U/g and the protein loading amount was 210.73 mg/g. Compared with free NHase, the optimum temperature of NHase@Co 3 (PO 4 ) 2 was 40 °C, which was higher than that of the free NHase (30 °C). The thermal, pH, antiproteolytic, and storage stability of NHase@Co 3 (PO 4 ) 2 were all improved. Furthermore, NHase@Co 3 (PO 4 ) 2 could be applied in the production of nicotinamide (NAM) with a satisfying yield and it could be reused seven times. All these results in this work clearly confirmed that the cobalt phosphate nanocrystals, as an original nanocarrier, would have promising applications for constructing nanobiocatalyst systems.