High-phosphorus manganese ores provide an important source of manganese, which is regarded as an irreplaceable material in the steel industry. The ammonia-ammonium carbonate leaching method was proposed for the removal of phosphorus and extracting manganese from high-phosphorus manganese ore, both effectively and environmentally. To explore the dissolution behavior of phosphorus and manganese in the ammonia-ammonium carbonate solution, the effect of the ammonia-to-ammonium carbonate concentration ratio, the leaching temperature, and the liquid-to-solid ratio on manganese extraction and dephosphorization rate were investigated. In addition, the composition of precipitated manganiferous sample, which was obtained from high-phosphorus manganese ores by ammonia-ammonium carbonate leaching process, was also studied. The results indicated that more than 99.2% phosphorus was removed and more than 83.5% of manganese was extracted by ammonia-ammonium carbonate leaching under the following conditions: ammonia to ammonium carbonate concentrations: 14:2 mol/L; liquid/solid ratio: 5:1 mL/g; leaching temperature: 25 °C; The precipitated manganiferous sample has little impurities, Mn% is 44.12%, P% is 0.02%, P/Mn = 0.00045.