The remelting of aluminum scraps can result in the accumulation of impurities, with iron being the most prevalent among them. The presence of such impurities can cause downgrading and hindered utilization of the material. Despite this, the evolution mechanism of the Iron-containing Intermetallic Phase (IIP) in recycled high-Fe and low-Si aluminum melt has received limited attention and requires further investigation. This study investigates the evolution mechanism underlying the precipitation behavior and organization of the IIP during the solidification process of recycled high-Fe Al-Zn-Mg-Cu melts, utilizing a combination of simulation and experiment. Our findings indicate that the precipitation behavior of the high-temperature precipitation phase (HPP) in the melt is influenced by the Mn and Si, which subsequently determines the organization of the IIP. Specifically, the predominant forms of IIP in the recycled high-Fe Al-Zn-Mg-Cu alloys are lamellar and hollow rod-like phases with anisotropic, as well as skeletal phases with isotropic organization. Moreover, the synergistic addition of Mn and Si can increase the precipitation temperature (PT) and precipitation temperature interval (PTI) of the Al15(Fe,Mn)4Si2 phase in the melt, leading to the transformation of the IIP into a skeletal organization that can be easily removed and has less impact on the material properties. These findings provide insights into alloy design strategies aimed at minimizing the impact of iron accumulation on the cycle life of aluminum scraps and the performance of recycled aluminum.