The conventional mechanoluminescence (ML) mechanism of phosphors such as SrAl2O4:Eu and ZnS:Mn is known to utilize carrier trapping at shallow traps followed by stress (or strain)-induced detrapping, which leads to activator recombination in association with local piezoelectric fields. However, such a conventional ML mechanism was found to be invalid for the ZnS:Cu-embedded polydimethylsiloxane (PDMS) composite, due to the absence of luminescence with a rigid matrix and a negligibly small value of the piezoelectric coefficient (d33) of the composite. An alternative mechanism, namely, the triboelectricity-induced luminescence has been proposed for the mechanically driven luminescence of a ZnS:Cu-PDMS composite.