Recently we demonstrated that CaAl2Si2O8: Eu2+ showed novel strong mechanoluminescence (ML). In order to improve the mechanoluminescence intensity, we partly substituted the Ca2+ ions by Sr2+ ions. It was found that the ML intensity was enhanced about three times as great as the one of CaAl2Si2O8: Eu2+ by substituting 40% of Ca2+ ions to Sr2+ ions. Furthermore it was revealed that the main peaks in XRD pattern shifted to lower angle side and the emission peak shifted to a short wavelength from 428 to 418 nm, indicating that the substitution resulted in the cell volume expansion and the change of luminescent color. Based on the results of thermoluminescence and electroluminescence measurements, the possible mechanisms for the improvement of ML intensity were proposed.