As Internet of Things-based technologies continue to digitalize our society, the development of secure and robust identification systems against evolving adversaries remains a grave challenge. Recently, physical unclonable functions (PUFs) have garnered tremendous scientific interest due to their intrinsic randomness, which makes them difficult to counterfeit. Herein, we present a facile approach for fabricating optical PUFs using spontaneous mirror symmetry breaking of molecular self-assembly. The PUF composed of racemic helical structures that generate chiroptical signals exhibits high encoding capacity (similar to 10(13 000)), precise recognition rate, and impressive reconfigurability. The present study demonstrates that the utilization of random symmetry breaking is a promising approach to the design of high-level security systems.