Against the backdrop of the global "carbon peaking and carbon neutrality" goals, as a field of high carbon emissions, the steel industry urgently needs to develop green and low-carbon metallurgy technologies to reduce carbon emissions. Electrolytic iron technology has emerged as a key research direction for low-carbon metallurgy, as it directly utilizes green electricity to drive reduction reactions and reduces fossil energy consumption associated with traditional blast furnace ironmaking. The sulfate-system electrolytic iron process exhibits promising industrial application potential due to its simplicity and low cost. However, the morphological control of iron deposits and impurity removal during electrolysis remain critical issues restricting its development. In this study, the preparation of electrolytic iron was conducted in a sulfate electrolyte system using an iron plate as the anode. The effects of electrolysis time (5~180 min), electrolysis temperature (20~80℃), Fe2+ concentration (20~100 g/L), current density (400~1200 A/m2) and cathode material (Ti, Cu, Ni, Al, Fe) on the morphology, purity, and current efficiency of electrolytic iron were systematically investigated. The results showed that the titanium cathode could significantly inhibit impurity introduction. Under the optimized conditions of an electrolysis temperature of 80℃, Fe2+ concentration of 60 g/L, current density of 1000 A/m2, and electrolysis time of 30 min, electrolytic iron products with excellent morphology and easy stripping were obtained. XRD, SEM-EDS, and dissolution analysis indicated that the as-prepared product was dominated by pure iron via synergistic regulation of multiple parameters. It exhibited a stepped morphology with clear grain boundaries, closely packed particles, and extremely few pores. The maximum purity achieved by spot scanning was 99.97wt%, and the iron purity measured by dissolution analysis was 99.94wt%. Under the optimized conditions, the current efficiency exceeded 97%, and the direct current consumption for electrolysis was approximately 4.35 kWh/kg-Fe. This research not only provides a technical path that has both cost-effective and performance advantages for the industrial production of electrolytic iron, but also provides theoretical basis and practical reference for the development of low-carbon metallurgy technology, which is of great significance to promoting the green transformation of the steel industry.