The work aims to reveal the atmospheric corrosion behavior of vermicular graphite cast iron (VGCI) and clarify the corrosion law and corrosion mechanism. Accelerated salt spray corrosion experiments were carried out in laboratory, and the results were characterized by weight loss, SEM/EDS, XRD and electrochemical methods. The cross section of VGCI had obvious stratification in neutral salt spray. The corrosion rate was 0.53 mg/(cm2×h) in the early stage, and then fluctuated in the later stage, but the overall stability tended to be 0.36 mg/(cm2×h). The corrosion potential (Ecorr) of the vermicular graphite cast iron rust sample decreased first and then increased from -680 mV to -600 mV, and the change trend of the polarization resistance (Rp) was consistent with the corrosion potential (Ecorr). The self-corrosion current (Icorr) had obvious fluctuations throughout the corrosion cycle and the corrosion products of VGCI in neutral salt spray were: Fe(OH)3, Fe2O3, FeOOH and a small amount of Fe3O4 as well as metal carbide Fe2C. VGCI can be developed into comprehensive corrosion after 84 h in neutral salt spray environment, with gully appearance and the microscopic appearance of corrosion products is shown in clusters and lamella. In the early stage of corrosion, an oxide film is formed on the surface of the matrix due to electrochemical corrosion, and the corrosive medium corrodes the matrix along the graphite to generate internal stress, resulting in the fracture of the outer rust layer. At the same time, the corrosion products on the worm-like graphite are in loose clusters. The two together forms the medium mass transfer channel, making the corrosion easier to develop.