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Octopus suckers offer remarkable adhesion performance against nonporous surfaces and have inspired extensive research to develop artificial adhesives. However, most of existing octopus‐inspired adhesives are either passive without an actuation strategy or active but not energy efficient. Here, a novel design of a magnetically actuated, energy‐efficient smart adhesive with rapidly tunable, great switchable, and highly reversible adhesion strength inspired by the elastic energy storage mechanism in octopus suckers is reported. The smart adhesive features two cavities separated by an elastic membrane with the upper cavity filled with magnetic particles while the lower one empty. The deformation of the elastic membrane can be actively controlled by an external magnetic field to change the cavity volume, thus generating a cavity‐pressure‐induced adhesion. Systematically experimental and theoretical studies reveal the fundamental aspects of design and operation of the smart adhesive and give insights into the underlying adhesion mechanisms. Demonstrations of this smart adhesive in transfer printing and manipulation of various surfaces in both dry and wet environments illustrate the potential for deterministic assembly and industrial or robotic manipulation. [ABSTRACT FROM AUTHOR]