Loose and uncemented calcareous sand slopes are prone to collapse under rainstorm erosion. In order to improve the erosion resistance stability of slopes, it is crucial to enhance the erosion resistance of calcareous sand. In this study, a new method of cementing calcareous sand with zinc sulfate solution (ZSS) is proposed. The ZSS reinforcement technique can effectively cement calcareous sand, enhance the mechanical properties and help reduce erosion on calcareous sand slopes. A series of laboratory experiments were conducted, including uniaxial compression tests, Brazilian splitting tests, surface penetration tests, microscopic tests, and rainfall scouring tests. The test results show that the uniaxial compressive strength of calcareous sand achieved 8.3 MPa reinforced with ZSS. Microscopic analyses revealed the mechanism of reinforcement, discovering the formation of environmentally friendly compounds such as ZnCO3 and CaSO4·2 H2O between calcareous sand particles, which enhanced the soil mechanical properties. The calcareous sand slope reinforced with ZSS forms a hard shell on the slope surface, which effectively improves the erosion resistance of the slope. After being reinforced with a ZSS concentration of 1.0 mol/L, the slope remained stable after 20 min of scouring at a rainfall intensity of 80 mm/h. This method provides a quick solution for reinforcing calcareous sand slopes and holds promising potential for practical engineering applications.