In this work, layered double hydroxide (LDH) and reduced graphene oxide (rGO) were incorporated into Zn/Ni matrix coating by cold-spraying on the surface of Mg alloys. Inside the resulting GLG@Zn/Ni coating, LDH/rGO are homogeneously dispersed and inner-connected to a protective network. Compared with other coatings without LDH or rGO nanosheets, the GLG@Zn/Ni coating shows the best corrosion resistance, with a high self-corrosion potential at − 1.174 V (vs. − 1.471 V for Mg), a decent self-corrosion current density of 344.7 μA·cm−2 (vs. 878.3 μA·cm−2 for Mg), and the longest available protection (>720 h) against corrosion. Electrochemical and morphological characterizations reveal a synergistic effect of the coating compositions in enhancing corrosion resistance. In detail, the LDH/rGO network inside the coating restricts the penetration of the corrosive medium, particularly for LDH, which has the capacity to capture corrosive Cl− ions. Meanwhile, Ni promotes the conversion of Zn into passivation layers, which then spread to fill the corrosion pores and interphase cracks. This transformation ultimately leads the GLG@Zn/Ni coating to become a unified whole, providing excellent corrosion resistance.