The effects of double-step homogenization processes on the precipitation of Al3Zr dispersoids and the dissolution of the primary phases of 2196 aluminum alloy were studied by optical microscopy, scanning electron microscopy (SEM), and transmission electron microscopy (TEM). It was revealed that first-step homogenization facilitates the nucleation of Al3Zr, while second-step homogenization results in the dissolution of the primary phases and the growth of Al3Zr dispersoids. The nanosized θ’ precipitates formed in the first-step homogenization are dissolved after the second-step homogenization. The optimum homogenization process was selected as 400 °C/10 h + 520 °C/24 h, which effectively dissolves the primary phases and promotes the formation of refined distribution of Al3Zr dispersoids. This phenomenon is mainly caused by the highest nucleation rate of the Al3Zr phase at 400 °C. While reducing the heating rate of the homogenization process can increase the number density of the Al3Zr dispersoids and reduce the precipitate free zone (PFZ), it does not alleviate the inhomogeneity of the Al3Zr precipitation. These results are expected to be meaningful for tailoring the industrial homogenization processing of as-cast Al-Cu-Li alloy.