We report the effect of Sr substitution on the crystal growth and piezoelectric properties of calcium magnesium silicate Ca2MgSi2O7 (CMS) single crystals. Strontium-substituted CMS single crystals with a chemical composition of Ca1−x
Sr
x
MgSi2O7 (CSMS100x; x = 0.0 to 0.6) were grown using the conventional Czochralski method. CSMS100x crystals without impurity phases are obtained up to x = 0.5. Both crystallographic axis c and a increased with the Sr content x, and the crystallographic axis ratio a/c decreased. The piezoelectric d
36 constants obtained using CMS, CSMS30, and CSMS40 crystals decreased with an increase in the Sr content x. Based on these observations, a relationship between piezoelectric properties and crystal structure was found using data from 14 types of melilite-type crystals. It was found that d
36 increases with an increase in a/c.