In this paper, effect of various contents of chitosan (1.0, 1.5 and 2.0 wt%) on corrosion/degradation behavior of ternary HA-NrGO-CS prepared on ZK60 alloy substrates were investigated. The samples were prepared by combining cathodic electrophoretic deposition and thermal argon atmosphere annealing for 120 min at 200 °C to regulate corrosion and quick degradation of ZK60 Mg alloy surface. After immersion for 30 min, HA-NrGO-1.5CS coated sample exhibited highest |Z|0.1Hz value, trailed by the HA-NrGO-2.0CS, HA-NrGO-1.0CS and ZK60 alloy samples. After immersion for 2 days, |Z|0.1Hz values moved to higher Bode modulus for HA-NrGO-CS coated samples, indicating poles and defects were filled due to the formation of apatite layer on the HA-NrGO-CS surface. FT-IR and Raman spectra proved the successful doping of N atoms into the rGO nanosheet skeleton to form NrGO. The SEM images and EDS plane-scan results for the samples after immersion for 2 days verified the existence of an apatite layer. The experimental results indicated that the existence of CS, HA and NrGO in the composite coatings can regulate the pH values and supply a sustained release of Mg2+ ions and O2 due to the synergistic effect of the protonation/deprotonation of -NH2 groups in CS and the dissolution/recrystallization of HA. Furthermore, the production of MgO2 film can convert corrosion behavior of ZK60 alloy from pitting corrosion to uniform corrosion, which provided a potential strategy for bone biomedical applications.