Stepped and Graded Peel Force Modulation in Patterned Liquid Crystalline Elastomer Adhesives

ABSTRACT Encoding local variations in the peel force response of pressure‐sensitive adhesives (PSAs) unlocks new functional possibilities for applications requiring both strong adhesion and facile, user‐directed detachment. Recent studies have demonstrated that liquid crystalline elastomers (LCEs) with monodomain planar orientation function as anisotropic adhesives, exhibiting direction‐dependent peel forces based on LCE alignment. Building on these findings, we investigate the ability to engineer peel force profiles through spatial patterning of director alignment. We systematically analyze adhesion of patterned LCEs with planar director orientation by varying spatial pattern frequency, polymer composition, peel velocity, backing stiffness, and adhesive thickness. LCE PSAs with both binary (stepped) and gradient (graded) patterning of orientation, and therefore peel force, are demonstrated. Our results establish design parameters that define the minimum resolvable pattern length scale, offering insights for tuning local adhesion contrast in LCE‐based PSAs.