The impact of zinc (Zn) on the seed decomposition process of sodium aluminate solution at different caustic concentrations was investigated. The results showed that as the concentration of Zn(II) in sodium aluminate solution increased from 0 to 1000 mg/L, the decomposition efficiency of the solution and average grain size of the resulting aluminum tri-hydroxide (ATH) changed little at a caustic concentration of 141 g/L. At caustic concentrations of 160 g/L and 177 g/L, the decomposition efficiency increased from 35.8% and 21.6% to 40.6% and 24.9%, respectively, while average grain size of the ATH crystal seeds increased from 14.2 and 9.25 μm to 17.9 and 15.9 μm, respectively. The XRD, FT-IR, and SEM analyses showed that zinc can enter the ATH seeds and interact with the α-ATH crystal planes. It may also form interactions with the AlO octahedral growth structure, thus promoting solution decomposition and influencing crystal growth. The research results will provide valuable references for improving the quality of alumina products.