The surface structures and properties of a membrane largely determine its in-service performance during a filtration process. Here we report a facile hydrophilization method via co-deposition of mussel-inspired polydopamine (PDA) and polyethyleneimine (PEI) on a polypropylene microfiltration membrane. The deposition time is greatly shortened and the surface hydrophilicity is significantly improved compared to those membranes decorated only by PDA. The dopamine/PEI deposition solution can be reused several times with negligible effect on the surface hydrophilicity of membranes. Moreover, the PDA/PEI coating endows the membranes with ultra-high water permeability, allowing microfiltration separation of oil-in-water emulsions under atmospheric pressure.