A novel afterglow mechanoluminescent (ML) composite elastic material was obtained with ZrO2:Ti4+ phosphor synthesized by a solid-state method and PDMS polymer. The structure, luminescence and traps properties of the phosphor and the elastomer were investigated by X-ray diffraction, scanning electron microscopy, and spectroscopy. The results show that ZrO2 belongs to a monoclinic system with a space group P21/c (No.14), which is a centrosymmetric structure, and its ML is irrelevant to the common piezoluminescence. The band gap of the matrix is 5.01 eV, and its width is large, which is conducive to the irradiation transition of the luminescence energy level. The cyan photoluminescence and afterglow luminescence with Ti4+ characteristic emission eg→t2g are obtained after Ti4+ is uniformly doped into ZrO2 as a luminescence center. After it is irradiated by 254 nm ultraviolet lamp, the composite elastic material prepared with ZrO2:Ti4+ phosphor and PDMS can emit bright cyan ML under the stimulation of external forces such tearing, pressing, bending and stretching.The ML occurs clearly for several seconds. The afterglow mechanoluminesascent phenomenon is linearly dependent on the stress and it can repeat after irradiation, indicating a promising application potential in the fields of stress visualization, force-light sensing, engineering detection and artificial skin. In addition, a possible mechanism of afterglow ML caused by triboelectricity induced trapped carrier excitation was also proposed.