Lead zirconate titanate (PZT) is a piezoelectric material that can sense or respond to mechanical deformations and can be used in ceramic electro‐mechanical systems (C‐MEMS). The microstructural, electrical, and piezoelectric characteristics of thick PZT films on low‐temperature cofired ceramics (LTCC) and alumina substrates were studied. The PZT composition was prepared with low‐melting‐point additives in order to decrease the sintering temperature and to be compatible with thick‐film technology. The integration of the PZT thick‐film materials on ceramic substrates could lead to degradation of the PZT's characteristics due to the interactions between an active PZT layer and a substrate, particularly with glassy LTCC material. To minimize the interactions with LTCC substrates, an intermediate PZT barrier layer was integrated. The value of the piezoelectric coefficient d₃₃ was found to be up to 120 pC/N on an alumina substrate and approximately 50 on an LTCC substrate. Based on these results, a cantilever‐type actuator was designed and fabricated on alumina substrates. Under an applied voltage of 200 V, the maximum tip deflection was about 5 μm.