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This review includes synthetic methods, characterization techniques, electronic structure-regulating strategies, and electromagnetic wave absorption applications of high-entropy materials. 

Abstract Nature provides many examples of the benefits of nanoscopic surface structures in areas of adhesion and antifouling. Herein, the design, fabrication, and characterization of liquid crystal elastomer (LCE) films are presented with nanowire surface structures that exhibit tunable stimuli‐responsive deformations and enhanced adhesion properties. The LCE films are shown to curl toward the side with the nanowires when stimulated by heat or organic solvent vapors. In contrast, when a droplet of the same solvent is placed on the film, it curls away from the nanowire side due to nanowire‐induced capillary forces that cause unequal swelling. This characteristic curling deformation is shown to be reversible and can be optimized to match curved substrates, maximizing adhesive shear forces. By using chemical modification, the LCE nanowire films can be given underwater superoleophobicity, enabling oil repellency under a range of harsh conditions. This is combined with the nanowire‐induced frictional asymmetry and the reversible shape deformation to create an underwater droplet mixing robot, capable of performing chemical reactions in aqueous environments. These findings demonstrate the potential of nanowire‐augmented LCE films for advanced applications in soft robotics, adaptive adhesion, and easy chemical modification, with implications for designing responsive materials that integrate mechanical flexibility with surface functionality.