Electrolytic manganese residue (EMR) from the electrolytic manganese industry is a solid waste containing mainly calcium sulfate dihydrate and quartzite. It is impossible to directly use the EMR as a building material due to some contaminants such as soluble manganese, ammonia nitrogen and other toxic substances. To immobilize the contaminants and reduce their release into the environment, treating EMR using alkaline additives for stabilizing manganese and removing ammonia was investigated. The physical and chemical characteristics of the original EMR were characterized by XRFS, XRD, and SEM. Leaching test of the original EMR shows that the risks to the environment are the high content of soluble manganese and ammonia nitrogen. The influence of various alkaline additives, solidifying reaction time, and other solidifying reaction conditions such as outdoor ventilation and sunlight, and rain flow on the efficiencies of Mn2+ solidification and ammonia nitrogen removal was investigated. The results show that with mass ratio of CaO to residue 1 : 8, when the solidifying reaction was carried out indoors for 4 h with no rain flow, the highest efficiencies of Mn2+ solidification and ammonia nitrogen removal (99.98% and 99.21%) are obtained. Leaching test shows that the concentration and emission of manganese and ammonia nitrogen of the treated EMR meets the requirements of the Chinese government legislation (GB8978-1996).