ZnS-based mechanoluminescent film has been widely used in the fields of stress visualization and stress sensing, due to its high brightness and repeatable stable luminescent characteristics. To evaluate the flexibleelastic deformation performance of ZnS-based mechanoluminescent film, both visual inspection and digital image correlation (DIC) are, respectively, employed for measuring the ZnS-based mechanoluminescent film. ZnS:Cu ²⁺ mechanoluminescent powders are first mixed with polydimethylsiloxane (PDMS) matrix to produce ZnS:Cu ²⁺–PDMS mechanoluminescent film. Then, two measurement experiments are, respectively, conducted to investigate the mechanical response and the flexible-elastic deformation performance of the prepared ZnS:Cu2+–PDMS mechanoluminescent film. On one hand, the mechanical response performance of the ZnS:Cu ²⁺–PDMS mechanoluminescent film is validated by visual monitoring of composite concrete fracture processes. On the other hand, the prepared ZnS:Cu ²⁺–PDMS mechanoluminescent film is also measured by DIC to obtain its full-field deformations and strains information. The flexible-elastic deformation performance of the ZnS:Cu ²⁺–PDMS mechanoluminescent film is well demonstrated by the DIC measured results.