The integration and the device realization of Pb(Zr, Ti)O3 (PZT) thick films on Si substrates are known to be extremely difficult because the processing temperature of the PZT thick film is close to the melting point of Si. However, PZT thick-film devices on Si warrant attention as they are appropriate for biological transducers; they generate large actuating forces and have a relatively high sensitivity for mass detection, especially in liquids. In this study, Pb(Zr0.52Ti0.48)O3 thick-film cantilever devices are successfully fabricated on a Pt/TiO2/SiNx/Si substrate using a screen-printing method and microelectromechanical systems (MEMS) process. Elastic and electromechanical properties such as the Young's modulus and transverse piezoelectric coefficient are determined from microstructural and electrical analyses for further mechanical study. The calculated Young's modulus of the thick film, 53.9 ± 3.85 GPa, corresponds to the resonant frequency obtained from the measured harmonic oscillation response. The transverse piezoelectric constant, d31, of –20.7 to –18.8 pC N–1 is comparable to that of a dense thin film. These values promise the possibility of determining the resonance properties of a thick-film cantilever by designing its structure and then simulating the harmonic oscillation response. Using the PZT thick-film cantilever, a strong harmonic oscillation with a quality (Q) factor of about 23 is demonstrated in water. The observation of strong harmonic oscillation in liquid implies the feasibility of precise real-time recognition of biomolecules using PZT thick-film cantilevers.