“…Owing to the characteristics of interfacial interactions between micrometer-to-millimeter surfaces, studies of the MSA mechanism are used to understand diverse non-covalent interfacial phenomena such as bio-/wet adhesion, 12,13 self-healing. 14−16 Meanwhile, MSA has been developed as a facile modular fabrication strategy to prepare heterogeneous structures, 17 bio-scaffolds, 18,19 actuators, 20 and information storage materials. 21−23 To extend the applicable scenarios of MSA, much progress has been achieved on enriching supramolecular interactions (molecular recognition, 1,24 hydrogen bonding, 8 electrostatic interactions, 25 DNA hybridization, 4,9 and so on), extending building block materials (gels, 1,4,[8][9][10]26 elastomers, 25,27,28 quartz, and metal 17 ) that could realize MSA, and revealing the assembly mechanism.…”