Novel hybrid coatings with excellent wettability are architecturally constructed on the surfaces of different types of separation membranes via simultaneous polymerization of mussel-inspired dopamine and hydrolysis of commercially available and low-cost silane through a highly efficient one-step approach. After coating with the designed hybrid coatings, the ultrafiltration (UF) membranes possess high hydrophilicity and excellent dry storage ability while the microfiltration (MF) membranes are endorsed with superhydrophilicity and underwater superoleophobicity. Such unique UF and MF membranes can be deployed for treating protein-rich water with drastically enhanced functions and separating oily water (oil-in-water emulsion) under atmospheric conditions with ultrahigh water flux and superior antifouling abilities. This versatile strategy to tailor membrane surface wettability paves the way for separation membranes to be used in harsh water environmental remediation and greatly stimulates the rapid development of mussel-inspired pDA based hybrid materials for advanced applications.