In this paper, olive-like ZnO particles were successfully synthesized via a facile biomineralization process in the template of silk fibroin (SF) peptide at room temperature. The coat of SF peptide on the surface of ZnO particles had a substantial influence on their morphology during the biomineralization. Room-temperature photoluminescence behavior of ZnO particles indicated that the visible blue emission peak centered at 410 run was enhanced with the mineralization time. Bacteriological tests revealed that the mineralized ZnO particles with SF peptide were not toxic for Staphylococcus aureus, Escherichia coli, and Streptococcus agalactiae, presenting good cytocompatibility due to the surface coal of peptide. Their potential applications in bio-optical detectors could be envisioned.