3D printing of flexible piezoelectric composites (3D-FPCs) is increasingly attracting the attention due to its unique advantage for customized smart applications. However, current research mainly focuses on the 0–3 piezoelectric composites, in which the piezoelectric ceramics are embedded in polymer matrix in the form of particles. The poor connectivity between particles much reduces the conduction of strain and charge in the composites, seriously limiting its application in actuation. In this work, a continuous lead zirconate titanate (PZT) double-layer ceramic scaffold was prepared by 3D printing and assembled with epoxy resin and interdigital electrodes together to manufacture a multifunctional device. The 3D-FPCs exhibit a free strain of 1830 ppm in actuating and are able to actuate a stainless-steel cantilever beam to produce a tip displacement of 5.71 mm. Additionally, the devices exhibit a sensitivity of 26.81V/g in sensing applications. Furthermore, 3D-FPCs are demonstrated as actuators for mobile small robots and wearable sensors for sensing joint activities.