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A recombinant protein ChiSifiCa, which was originally designed for regulation of calcium carbonate, was utilized to direct the mineralization of PbI2. By the regulation of ChiSifiCa protein, PbI2 nanoparticles composed of crystalline nanoflakes and amorphous nanorods were fabricated under environmental benign conditions. Synthetic PbI2 was successfully applied for preparation of perovskite precursors to fabricate solar cells. This regulation of ChiSifiCa on PbI2 improves the power conversion efficiency of corresponding perovskite solar cells to 16％. The present study may open a new avenue in the design and synthesis of materials with novel structures and functions.