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We have investigated the processing of lead-zirconate-titanate-based thick films by inkjet printing Pb(Zr0.53Ti0.47)0.98Nb0.02O3 with a 6 mol% excess of PbO nanosized powder dispersed in water. Different waveforms were employed to determine the optimum size and shape of the drops. A uniform, defect-free pattern with dimensions of 4 mm × 4 mm can be printed using 20 V and a drop spacing of 20 μm. The inkjet-printed films were heated to 400 °C to remove the organics and subsequently sintered at 750 and 850 °C. The correlations between the density, grain size and electromechanical properties of the thick films and bulk ceramics are qualitatively discussed. A thickness coupling factor of 46% was obtained for a 15-μm-thick film sintered at low temperature of 850 °C, which is comparable to the value of the bulk ceramic with an identical nominal chemical composition. Our results are important for the economic and environmental-benign printing of piezoelectric materials applicable in variety of electronic devices, such as sensors, actuators, transformers, piezoelectric energy harvesters and transducers.