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Dopamine is a “sticky” biomolecule containing the typical functional groups of mussel adhesive proteins. It can self-polymerize into a nanoscale thin film on various surfaces. We investigated the surface, adhesion, friction, and cracking properties of polydopamine (PDA) thin films for their effective transfer to functional devices and biocompatible coatings. A series of surface characterizations and mechanical tests were performed to reveal the static and dynamic properties of PDA films coated on glass, polydimethylsiloxane (PDMS), and epoxy. We found that PDA films are highly hydrated under wet conditions because of their porous membrane-like nanostructures and hydrophilic functional groups. Upon dehydration, the films form cracks when they are coated on soft substrates due to internal stresses and the large mismatch in elastic modulus. The adhesive pull-off force or the effective work of adhesion increased with …