Aqueous zinc-ion batteries are highly favored for their enhanced safety and reduced cost. However, there exist challenges including zinc dendrite, hydrogen evolution, and surface corrosion to be solved. Using electrolyte additives is a highly convenient approach to solving zinc anode-related issues. Inspired by industrial corrosion protection, a trace amount of the corrosion inhibitor urotropine (URT) is used as an electrolyte additive to protect the zinc anode. Theoretical calculation and experimental analysis confirm the adsorption of URT molecules onto the surface of Zn, which inhibits hydrogen evolution. This adsorption further leads to the formation of an inorganic-organic bilayer solid electrolyte interface (SEI) on the surface of the zinc anode, effectively protecting the Zn anode from corrosion, hydrogen evolution and zinc dendrites. The presence of SEI enables symmetrical Zn//Zn cells to exhibit a long cycling performance of 1750 h at 1 mA/cm2 and an average coulombic efficiency of 99.0% at 1 mA/cm2 in Zn//Cu cells. After being coupled with polyaniline (PANI), the Zn//PANI full battery displays excellent cycle stability and specific capacity.