Carbon and oxygen-rich corrosion barrier layer formed on Mg by a simple and scalable CO2 atmospheric plasma (CO2-AP) process. The reactive CO2-AP interacts with the Mg surface and forms a unique layered structure with the top MgCO3/MgO-intermixed particulates pillars and the bottom dense layer. The surface features were simultaneously formed on the nano-/micro-structured MgO layer by carbonate molecules, plasma-active CO2 molecules, and/or other volatile organic compounds on the nano-/micro-structured MgO particle layer. The resulting surfaces after CO2-AP were either hydrophobic or hydrophilic and exhibited lower anodic current or high resistance for Mg corrosion. For the hydrophobic surfaces of CO2-AP treated Mg, molecular dynamic simulations were performed to understand the origin of hydrophobicity and identified that the amorphous carbon layers formed on the Mg surface are the source. The environmentally benign abundant-gas-based process enables the cost reduction associated with waste treatment, generation of by-product, and supply of raw material.