Piezoelectric materials have been developed since early 1900s and many research had been conducted on the composition and process to obtain higher piezoelectric constants ( d33 ). Within composition research, lead perovskite relaxor piezoelectric single crystals (SCs) of Pb(Mg1/3Nb2/3)O3-lead titanate PbTiO3 type have been actively studied since 1990s because of their outstanding pC/N compared with those of the conventional Pb(Zr,Ti)O3 ceramics. A major driving force of these SC research has been promoted by mass production of ultrasound transducers and array probes for medical diagnostic systems since early 2000s. However, higher d33 material and process research for these ultrasound devices are almost saturated. In this review article, we present a brief overview of the history, current situation, and future perspective of piezoelectric SCs. The authors believe that the main research in the next century is high d33 SCs with a high composition uniformity and low-energy SC growth methods, such as solid-state SC growth, low-loss SC transducer manufacturing technique, and improved poling process. This is a big technical challenge for all the scientists; however, the relatively large market of medical ultrasound has been expanded year by year, and we hope that the community is motivated to solve such technical problems in the near future.