Circularly polarized luminescent (CPL) materials have emerged as new advanced optical and photonic materials. While many efforts have been devoted to the organic CPL materials, it still remains a challenge to fabricate CPL active inorganic materials due to the difficulty in the introduction of the chiral units. Here, a simple approach for achieving CPL active inorganic persistent phosphor materials is reported. By modifying the inorganic persistent phosphor materials with enantiomeric cysteine via ball milling, the inorganic circularly polarized phosphorescence (CPP) materials with long afterglow characteristics are fabricated. Moreover, the circular polarization of the obtained phosphorescent materials can be controlled by the molecular chirality of the cysteine. The dissymmetry factor (glum) of the CPP materials can be up to 10−2. It is envisaged that this approach will afford a new insight into the designing of the inorganic functional chiral phosphorescent materials.