Low-temperature plasma polymerization is a promising alternative technique in creation of environmentally friendly coating systems for metallic corrosion protection. In this study, a DC low-temperature plasma technique, including plasma treatment and plasma polymerization, was used to create interface engineered coating systems with a structure of Mg/plasma interlayer/cathodic electrocoating (E-coat) for a magnesium (Mg) alloy AZ31B. The plasma interlayer deposited from trimethylsilane (TMS) precursor had a nano-scale thickness of ~ 65 nm and its surface properties was well-controlled by subsequent plasma treatments in order to achieve different level of interfacial adhesion between the E-coat and the Mg substrates. The surface wettability of the plasma interlayer was monitored by surface contact angle measurement. The interface adhesion of the coating system was evaluated using N-methylpyrrolidinone (NMP) paint removal test and ASTM tape test conducted under dry and wet conditions. Electrochemical impedance spectroscopy (EIS) was employed to investigate the effects of plasma interlayer properties including surface wettability and adhesion enhancement on corrosion protection properties of the coating systems to AZ31B Mg alloy. It was found that a more wettable interface enhanced the electrolyte penetration through the coating and thus reduced the corrosion resistance of the coating system. The detailed results obtained through this study will be presented and discussed.