In this study, we successfully prepared red‐emitting AlN:Mn2+ spherical phosphors by using nitrogen pressure–assisted carbothermal reduction–nitridation method. The optimum preparation parameters were explored by changing nitrogen pressure, CaF2 content, reaction temperature, and the amount of MnCO3. It was confirmed that uniform spherical shape, large particle size, less impurity content, and suitable Mn2+ concentrations could effectively enhance the luminous intensity of AlN:Mn2+ phosphors. The structural compositions of the AlN:Mn2+ phosphors were characterized by X‐ray diffraction and X‐ray photoelectron spectroscopy, indicating that Mn2+ ions were successfully doped into AlN lattice by substitution of Al3+ ions, thus providing the red‐emitting luminescence centers. Based on the experimental results, we further proposed the underlying growth mechanism of spherical AlN phosphors. It was suggested that an adequate amount of liquid Ca‐aluminates was essential to achieve uniform spherical morphology and high fluorescence efficiency.