From cell membrane to epidermis, growth-induced wrinkles and creases that originate in mechanical forces operating on multilayered structures are frequently observed in living organisms. [11] The biomimetic reproduction of similar structures has been achieved by driving the surface instability of polymeric materials, realizing the development of smart surfaces for use in dry adhesion, [12] sensors, [13,14] smart windows, [15] the patterning of biomaterials, [4,16] and cell cultures. [17,18] Although many studies have elucidated the mechanism of surface instability and thereby the formation of creases and wrinkles on elastomeric materials, [11,19] the precise engineering of surface instabilities remains an important challenge. Wrinkling and creasing can be engineered to control the surface topology of a polymer. The use of layered films consisting of soft substrate and rigid thin film has been widely studied with the aim of triggering modulus mismatch within a material. For example, metal deposition [19] or plasma treatment [20] can lead to the elastic substrate-derived spontaneous formation of random surface topology as a result of the mechanical stress caused by the thermal expansion of the materials. By controlling the thickness, the modulus of the materials, and post-processing conditions, the wavelength of wrinkle and crease structures can be controlled. The aforementioned methods have also been conducted on a prestrained substrate, enabling the formation of ordered 1D or 2D structures. [21-24] However, the surface topology of these materials is irreversible, limiting the dynamic control of such structures. Hydrogel films with cross-linking gradients have therefore been proposed for the production of dynamic and stimuli-responsive surface topologies. Recently, the osmotic pressure-driven surface instability of hydrogels was analyzed and used for the formation of long-range ordered surface topologies. [11,25] This strategy was further developed in an attempt to control the characteristic size and shape of the surface topology in order to form pre-defined surface patterns combined with a lithographically patterned structure. [26] However, highly uniform surface patterns were not generated because osmotic pressure-driven swelling was found to occur simultaneously over the entire area. In addition, the omnidirectional propagation of the surface patterns inevitably led to disorder in the surface patterns. The creases and wrinkles that form on soft matter have been comprehensively analyzed and engineered to utilize their topological advantages in various research fields. Although the principle for the formation of such structures is found to be the inhomogeneous distribution of mechanical stress, simultaneous and omnidirectional propagation of surface patterns makes it difficult to engineer these structures. A design strategy for the reversible formation of highly uniform crease patterns on hydrogel films is proposed by driving the stepwise evolution of creases. A hydrogel film with a smooth-and submicron-scale sur...