This work investigates symmetry-breaking deformation of azo molecular glass microspheres induced by interfering circularly polarized light, and related particle shape manipulation as well as 3D patterning. The isolated microspheres and microsphere monolayers are obtained from an azo molecular glass (IA-Chol) by the solution dispersion method and soft-lithography, respectively. Unique symmetry-breaking deformation is observed for the microspheres upon exposure to the spatially modulated light field, which is produced by interference of two orthogonally polarized laser beams with the right-circular polarization (RCP) and left-circular polarization (LCP). Two distinct deformation modes are developed upon the irradiation with the interfering beams in RCP:LCP and LCP:RCP superposition manners, respectively. The unique morphologies with the symmetry-breaking characteristics are caused by mass transfer induced by the light irradiation. For the microsphere monolayers, the deformations of the microspheres not only capture and record the polarization states of the light field, but also create various surface patterns combining the symmetry-breaking deformations and periodic surface modulation. A variety of unique surface patterns are obtained by irradiation with the interfering circularly polarized waves with the orthogonal and also the same-handed polarizations. The material and methodology developed in this study are promising for applications in sensing, optics, responsive surfaces, and others.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201806703. dichroism (CD) spectroscopy, [4,5] quantumbased optical computing and information processing, [6,7] and all-optical magnetic recording with circularly polarized light, [8] to unmentioned others. As conventional semiconductors lack intrinsic chirality, the handedness of CPL cannot be distinguished and directly detected by ordinary photodetectors. Recently, materials and devices with selective responses to the handedness, such as chiral organic semiconductor transistor, chiral plasmonic metamaterials, and others, [9,10] have been developed for the CPL detection. Compared with conventional methods such as temporal modulation, ellipsometry, and others requiring specific optical set-ups, [11] the approaches based on the newly developed materials show advantages of being highly compatible with various photonic platforms without additional optical elements. Despite the wide-spread use of CPL and interest in its interaction with matter, it has scarcely been reported to use nonchiral material through shape deformation of the substances to capture and store the chirality of the electromagnetic wave. Distinct from the available usages and studies, such a research will not only supply a new method to distinctly detect polarization states of CPL through microscopic observations, but also pave a way toward shape manipulation and three-dimensional (3D) surface patterning with the light.In recent years, photoinduced mass...