LAUSR

Liquid crystal elastomers (LCEs) exhibit extraordinary energy dissipation due to their unique viscoelastic response, resulting from the rotation of mesogens under mechanical stress. While recent studies demonstrate the LCE‐based pressure‐sensitive adhesives (PSAs) by exploiting the enhanced damping, all previous studies have focused on LCEs with covalent crosslinks. Here, a new class of PSAs is developed by integrating movable polyrotaxane crosslinkers into an LCE matrix (PRx‐LCEs). Dynamic viscoelastic measurements reveal that PRx‐LCE exhibits a remarkably high energy dissipation, as indicated by a large tan δ. Interestingly, the secondary tan δ peak associated with LCE damping is more pronounced than the primary peak of the glass transition. The exceptional energy dissipation in PRx‐LCE results in superior adhesion strength (≈1864 N m−1), which is 3.5 times higher than conventional LCEs and 13 times higher than commercial PSAs in the peel test. Additionally, PRx‐LCEs demonstrate thermally reversible adhesion, enabling clean removal at elevated temperatures. Furthermore, the sliding effect in PRx‐LCE enhances both deformability and stress relaxation under load, resulting in deeper indentation, and superior adhesion during the probe tack test. The combination of LCE and slidable crosslinks provides robust and switchable adhesion, making them promising for applications in biomedical engineering, display, and semiconductor industries.