Many polymer materials can respond to external stimuli, so their surface topographies can be regulated in order to achieve specific functions, such as fabrication of lens arrays, control of cell adhesion, and manipulation of object movement. Among them, liquid‐crystalline polymers are the most promising because their unique properties of self‐organization, molecular ordering, and physical anisotropy enable themselves to generate complicated deformation when external stimuli are applied. Here, this work focuses on the principle of topographical deformation of liquid‐crystalline polymers induced by various external stimuli, giving some examples about how to modulate these surface patterns. Accordingly, potential applications of switchable surface topography are presented in the field of photonics, biology, and mechanics. Finally, the existing problems are proposed and future directions in this topic are given an outlook. This review is anticipated to offer new insights and guidelines for developing stimuli‐responsive polymer materials with broader applications.

Surface morphing of organic materials is necessary for advances in semiconductor processing, optical gratings, anticounterfeiting etc., but it is still challenging, especially for its fundamental explanation and further applications like advanced anticounterfeiting. Here, we report one strategy to acquire surface deformation of the liquid-crystalline azopolymer film using a two-step method: selective photoisomerization of azopolymers and then solvent development. In the first step, surface tension of the polymer film can be patterned by the selective photoisomerization of azopolymers, and then in the second step, the flowing solvent drags the underlying polymer to transport, leading to the formation of surface deformation. Interestingly, the direction of mass transport is opposite to the traditional Marangoni flow, and the principle of solvents’ choice is the matching of surface tensions between the azopolymer and the solvent. The two-step method shows characteristics of efficient surface morphing, which could be applied in advanced anticounterfeiting by the way of photomask-assistant information writing or microscale direct writing, and then reading in a specific liquid environment. This paves a new way for understanding the mechanism of mass transport toward numerous unprecedented applications using various photoresponsive materials.