The hydrothermal treatment followed by a self-assembled monolayer (SAM) of 1-butylphosphonic acid through the tethering by aggregation and growth (T-BAG) method was employed to produce protective surface coatings on the Mg-6Al-1Zn alloy (AZ61) for reducing the degradation rate in physiological environments. Potentiodynamic polarization measurements revealed that the organic self-assembled monolayer and Mg(OH)2 coating can further enhance the surface chemical stability and corrosion resistance of Mg alloys. SAM-treated Mg(OH)2 coatings can be served as a more passive surface layer as a result of their much higher charge transfer resistance and the presence of Warburg impedance in electrochemical impedance spectroscopy measurement.