LAUSR

Adhesion occurs by covalent bonding, as in reactive structural adhesives, or through noncovalent interactions, which are nearly ubiquitous in nature. A classic example of the latter is gecko feet, where hierarchical features enhance friction across the contact area. Biomimicry of such structured adhesion is regularly achieved by top-down lithography, which allows for direction-dependent detachment. However, bottom-up approaches remain elusive given the scarcity of building blocks that yield strong, cohesive, self-assembly across multiple length scales. Herein, an exception is introduced, namely, aqueous dispersions of cellulose nanocrystals (CNCs) that form superstructured, adherent layers between solid surfaces upon confined evaporation-induced self-assembly (C-EISA). The inherently strong CNCs (EA > 140 GPa) align into rigid, nematically ordered lamellae across multiple length scales as a result of the stresses associated with confined evaporation. This long-range order produces remarkable anisotropic adhesive strength when comparing in-plane (≈7 MPa) and out-of-plane (≤0.08 MPa) directions. These adhesive attributes, resulting from self-assembly, substantially outperform previous biomimetic adhesives obtained by top-down microfabrication (dry adhesives, friction driven), and represent a unique fluid (aqueous)-based system with significant anisotropy of adhesion. By using C-EISA, new emergent properties will be closely tied with the nature of colloids and their hierarchical assemblies.