laser processing methods are laser direct writing (LDW) and interference lithography (IL). [7][8][9] LDW utilizes a focused laser spot to write designed patterns through effects such as laser heating, photochemical reactions, ablation, etching, and plasma formation. [6,7] On the other hand, IL is accomplished by recording the interference patterns in a photoresist, where the single or multiple optical exposures produce straight lines, curves, dots, hollows, and various other structures. [8,9] More specialized methods have also been developed to go beyond the optical diffraction limit for laser precision engineering, which include the laser-processing in near field, laser-particle lithography, plasmonic nanolithography, multiphoton lithography, block-copolymer lithography, and others. [7,10] An unexpected observation and discoveries of laser-induced periodic surface structures (LIPSS), often termed ripples, have led to another new approach with various applications. [11,12] LIPSS was originally observed as weird surfacerelief periodic lines on solids after laser radiation. [13,14] Later studies found that these structures can be generated on almost every type of material (metals, semiconductors, and dielectrics) upon irradiation of pulse lasers with durations down to a few femtoseconds, where the formed patterns show close correlation with the wavelength and polarization of the radiation. [11,[14][15][16][17] The universal and intriguing nature of LIPSS has triggered remarkable research enthusiasm to understand its mechanism. [11,[18][19][20] As the ripple sizes are much smaller than the spot area, LIPSS can be used for nanoscale surface patterning and other applications. [12] Although LIPSS as a unique surface pattering method is widely explored with many interesting developments, the patterns formed through this approach are more or less limited to ripples and most of them are produced by expensive ultrafast pulse lasers.Azo polymers and azo molecular glasses (polymers and molecular amorphous materials containing azo chromophores) represent a fascinating class of photoresponsive materials, which have been intensively investigated for the fabrication of various surface patterns. [21][22][23][24][25][26][27][28][29][30][31] Among the first cases of the developments, surface-relief-gratings (SRGs) were inscribed on azo polymer films by exposure to interfering patterns of laser beams. [32,33] In contrast to the irreversible patterns obtained by A new approach to fabricate ordered complex surface patterns is established upon linearly polarized light (LPL) irradiation with a continuous wave laser. Distinct from typical laser-induced periodic surface structures, the ordered patterns are formed through unique topographical transitions of submicrometer pillar arrays of an azo molecular glass, when irradiated with LPL at 532 nm. As revealed by microscopic investigation and optical simulation, the structure formation results from the deformation of the original pillars along the electric vibration direction of LPL and grow...