The effects of Cr and Ni content on the low-temperature toughness and supercritical CO2 corrosion resistance of high-strength low-alloy steel (HSLAs) were investigated by optical microscopy, scanning electron microscope, electron backscattered diffraction, transmission electron microscope, X-ray Photoelectron Spectroscopy, electron probe X-ray micro-analyzer, critical crack tip opening displacement, and supercritical CO2 corrosion experiments. In this study, the complex structure of high-strength low-alloy steel is identified and quantified, and related to the critical crack tip opening displacement (CTOD). The further addition of Ni and Cr promotes the formation of granular bainite (GB) and martensite-austenite (MA). The proportion of high-angle grain boundaries in the GB structure is small and does not significantly hinder crack expansion, while MA frequently leads to the initiation and expansion of cracks, deteriorating the low-temperature toughness of the material. Supercritical CO2 corrosion experiments displayed that further addition of Cr and Ni will improve the density and protection of corrosion products. But high-density dislocations will destroy the integrity of the lattice structure of the material and may serve as diffusion channels to affect the formation of the passivation layer and repair. Moreover, dislocation-dense areas are more likely to capture impurity elements, forming a micro-battery effect and accelerating local corrosion. This reduces the extent to which Cr and Ni alloy elements improve the corrosion resistance of HSLA steel.