The development of fully solution-processed, biodegradable piezoelectrics is a critical step in the development of green electronics towards the worldwide reduction of harmful electronic waste. However, recent printing processes for piezoelectrics are hindered by the high sintering temperatures required for conventional perovskite fabrication techniques. Thus, a process was developed to manufacture lead-free printed piezoelectric devices at low temperatures to enable integration with eco-friendly substrates and electrodes. A printable ink was developed for screen printing potassium niobate (KNbO3) piezoelectric layers in microns of thickness at a maximum processing temperature of 120 °C with high reproducibility. Characteristic parallel plate capacitor and cantilever devices were designed and manufactured to assess the quality of this ink and evaluate its physical, dielectric, and piezoelectric characteristics; including a comparison of behaviour between conventional silicon and biodegradable paper substrates. The printed layers were 10.7–11.2 μm thick, with acceptable surface roughness values in the range of 0.4–1.1 μm. The relative permittivity of the piezoelectric layer was 29.3. The poling parameters were optimised for the piezoelectric response, with an average longitudinal piezoelectric coefficient for samples printed on paper substrates measured as d33, eff, paper = 13.57 ± 2.84 pC/N; the largest measured value was 18.37 pC/N on paper substrates. This approach to printable biodegradable piezoelectrics opens the way forward for fully solution-processed green piezoelectric devices.