The treatment with hydrofluoric acid (HF-treatment) was suggested to be an effective way of improving the corrosion resistance of Mg alloys, including Mg-Zn-Ca (ZX) ones used for biodegradable implants. However, the effect of the HF-treatment on the stress corrosion cracking (SCC) susceptibility of ZX alloys has not been reported yet, although this phenomenon can induce premature brittle failures of the metallic medical devices, and thus, it is critical for their in-service structural integrity. In the present study, the effect of the HF-treatment on the microstructure, cytotoxicity, corrosion rate, mechanical properties, and fracture and side surface characteristics of the as-cast ZX20 alloy were investigated with the use of scanning electron microscopy, immersion, and slow-strain rate tensile testing in Hanks’ solution and indirect cell viability tests. It is found that the HF-treatment exerts no cytotoxic effect and results in a significant reduction in corrosion rate (up to 6 times of magnitude) and SCC susceptibility indexes (up to 1.5 times of magnitude). The observed improvement of corrosion and SCC performance of the alloy by the HF-treatment is found to be attributed to three effects, including (i) formation of the protective surface film of MgF2, (ii) removal of surficial contaminations originating from sample preparation procedures, and (iii) dissolution of surficial secondary phase particles. The mechanism of corrosion and SCC in the specimens before and after the HF-treatment are discussed.