Various hydrogel actuators have been developed so far, however, their actuation has inherent limitation in efficiency, because of their primitive actuation mechanism simply relying on the volume changes through the swelling and deswelling of gel networks. These limitations could be overcome through the imitation of mechanisms shown in Nature’s living creatures, offering an enormous potential for the development of functional soft materials that may improve our life. As represented by muscular tissues, some biological tissues are composed of numerous nanoscopic subunits that are assembled into anisotropically oriented structures extending over amacroscopic size regime. To address this challenge, we have recently developed polymer networks with 'single-crystal-like'structural order, where 2D-shaped inorganic materials were employed as constituents. In this presentation, their unprecedented functions originating from anisotropic structures will be discussed.