In this study, three new Schiff bases were synthesized from paeonol and amino acids to prepare a compound Schiff base coating on the Mg-Zn-Y-Nd alloy (ZE21B alloy) surface by electrostatic spraying, and these three single Schiff base coatings were prepared on the ZE21B alloy as control. The results of SEM and XPS confirmed the successful preparation of the coating. Immersion tests and electrochemical tests showed that both the single coating and the compound coating significantly improved the corrosion resistance of ZE21B alloy, and the compound coating could play a synergistic corrosion inhibition effect, thus showing the best corrosion resistance.