Little is known why illumination of linearly polarized continuous‐wave laser light can induce gyrotropy (optical rotatory power) and macroscopic circular/screwing deformations in amorphous As2S3. Gyrotropy appears through scattering and deflection of the incident light in combination with negative photoinduced birefringence. The gyrotropy could also trigger atomic motions under photoinduced fluidity, which produces macroscopic deformations.