Recently, we have developed crystal-oriented sheet forming (COSF) process from green sheet process and high-magnetic-field method. We formed c-axis-oriented (Sr,Ca)2NaNb5O15 (SCNN) sheets by the COSF process, and succeeded in realizing c-axis-oriented single-plate type piezoelectric ceramics (O-SP) and c-axis-oriented multilayered type piezoelectric ceramics (O-MLPC) for SCNN. From the measurement results of displacement induced by electric field, it was clarified that effective d33 of the O-SP was 210~240 pm/V. This value was about 3 times larger than that of the randomly oriented single-plate type, which was 70% of that of single crystal. Moreover, it was confirmed that O-MLPC indicated displacements 2.5 times as large as that of the conventional multilayer piezoelectric ceramics. In this study, we clarified that piezoelectric properties in bulk and multilayer structure can be drastically enhanced using the COSF process.