An excellent cycle life (150 cycles with 80% retention) for lithium-metal anodes in lithium-ion batteries is achieved by employing mussel-inspired polydopamine-treated-polyethylene separators. This originates from the polydopamine coating, which enables a uniform ionic flux, as well as mussel-inspired catecholic adhesion of the separators onto the lithium surfaces. Additionally, the polydopamine coating improves the thermal-shrinkage properties of polyethylene separators.