Physiological human fluid is a natural corrosive environment and can lead to serious corrosion and mechanical damages to light Mg–Al alloys used in prosthetics for biomedical applications. In this work, organic–inorganic hybrid coatings doped with various environmentally friendly and non-toxic corrosion inhibitors have been prepared by the sol-gel process for the corrosion protection of AZ61 magnesium alloys. Effectiveness has been evaluated by pH measurements, optical microscopy, and SEM during a standard corrosion test in a Hanks’ Balanced Salt Solution. The results showed that the addition of an inhibitor to the sol-gel coating can improve significantly the corrosion performance, being an excellent barrier for the L-cysteine-doped hybrid sol-gel films. The incorporation of TiO2 nanoparticles, 2-Aminopyridine and quinine organic molecules slowed down the corrosion rate of the Mg–Al alloy. Graphene oxide seemed to have the same response to corrosion as the hybrid sol-gel coating without inhibitors.