We present a relationship between piezoelectric property and crystal structure in melilite-type crystals. Two independent piezoelectric constants, d 14 and d 36 , increase and decrease with the polyhedral distortion, respectively. Based on this knowledge, single crystals made of strontium-substituted calcium magnesium silicate Ca 2 MgSi 2 O 7 (CMS) have been submitted to the Czochralski method, which made them grown. The CMS crystal has a high d 36 ; however, its transition temperature is around 85°C. Therefore, the strontium substitution is conducted to decrease this phase transition temperature. A single crystal of strontium substituted CMS, with nominal chemical composition Ca 1.7 Sr 0.3 MgSi 2 O 7 (CSMS30), shows no phase transition when temperature rises from room to melting temperature. Its piezoelectric d¤ 31 constant is 2.1 pC/N and its compressive strength is 830 MPa on crystal substrate with (ZXt)45°cut. The CSMS30 single crystal is a superior candidate material for pressure sensors at high operating temperatures.