Jarosite precipitation process (JPP) is the most frequently used procedure for iron removal in the hydrometallurgical zinc extraction process. However, there is a gap in the knowledge of the relationship between operational parameters and the low contaminant JPP on the industrial scale. This study will address these issues by investigating the behavior of zinc calcine (ZC) as a neutralizing agent, exploring the source of zinc and iron through leaching experiments, and simulating the Jarosite process of the Bafgh Zinc Smelting Company (BZSC). The results showed that the zinc dissolution efficiency was 90.3% at 90 °C, and 73% of the iron present in the calcine can be solubilized. The main outcome was the iron removal of about 85% by alkaline ions present in ZC without the addition of any precipitating agent. The second target was to evaluate the effect of operational parameters on jarosite precipitation. Results revealed that increasing the temperature to 90 °C and the stirring rate to 500 RPM as well as adjusting the ZC’s pH during the jarosite precipitation remarkably improved iron removal. Considering all these factors in the plant could improve Fe precipitation to around 80% on average.