stimuli, including thermal, pH, electric, chemicals, etc. [3] Many of them rely on the interfacial properties of the contact, such as surface topography and chemical functionality. The former directly affects the contact area A to be detached and, therefore, the adhesion can indeed be altered by changing the surface topography. [4][5][6][7] The latter mainly affects the interfacial energy density via the bare surface tension of each material or chemical/physical bond/ entanglements. [8][9][10] However, less attention has been paid to the use of the bulk viscoelastic characteristics that are especially important in dynamic applications toward stimuli-responsive adhesives. [11,12] To our knowledge, no experimental study exists of the switchable adhesion of the nematic liquid crystal elastomers (LCEs), which possess unique bulk mechanical properties.LCEs are a unique class of elastomers, in which the nematic director is coupled to the polymer network in both static and dynamic manner. [13] In the macroscopically nonaligned LCE (called "polydomain"), the local uniaxial nematic order Q(T) develops in a usual manner of the frustrated first-order phase transition from the isotropic phase, [14] but the nematic regions of a characteristic size of a micrometer are randomly misaligned in the bulk material. As a result, the polydomain LCE is macroscopically isotropic, [15] but retains all its characteristic nematic LCE parameters (such as the elastic modulus and loss factor, both relevant to this study). In contrast, the aligned ("monodomain") nematic LCE shows the uniform macroscopic anisotropy Q(T) across the whole sample, and the characteristic effect of spontaneous shape change [16,17] on increasing temperature T across the nematic-isotropic transition temperature, T NI (often called "thermal actuation"). This effect makes LCE highly attractive for applications [13,[18][19][20][21][22] involving soft actuators, shape-memory materials, and others.The other unique characteristics of nematic LCE, on which we especially focus here, is the effect of "soft elasticity," which in dynamic-mechanical setting manifests itself in a large increase in the loss factor tanδ, and the decrease in the storage moduli E′ and G′. [13,[23][24][25] This effect shows a great potential in LCE as energy damping materials. [23,26] The higher internal viscosity originates from the additional nematic (orientational) interaction between polymer chains. This adds resistance against the local rotation of the liquid crystalline director relative to the network in response to the finite strain rate (similarly to the higher viscosity in the ordinary liquid crystals).