Electromechanical energy demands homogenous thick films of piezoceramics with sufficiently large piezoelectric constant and reproducible performance. Single-phase LiTaO 3 films deposited by sol-gel processing have been fabricated as cantilevers to investigate the interdependence of dielectric and piezoelectric properties as a function of film thickness. Phase pure LiTaO 3 films with varying thickness in the range of 2.07-4.37 µm on stainless steel substrates were obtained after calcination of samples at Accepted Article This article is protected by copyright. All rights reserved 650 °C. The relative permittivity of optimized spin-coated films peaked at 479.73 (1 kHz), whereas the piezoelectric coefficient (d 33 mode) determined by piezo force microscopy was in the range of 21-24 pm/V. The effect of poling was studied through the butterfly and phase curves. A figure of merit up to 3.29 (10-18 m 2 /V 2) was determined for cantilever devices, which were able to generate a peak-to-peak voltage of 0.046-0.15 V using a 1 MΩ resistor as an impedance load at a fixed acceleration of 1.5 m/s 2. While the power density was in the range of ~ 4-20x10-9 W/m 3 , increased with the increasing film thickness. The leakage current density decreased in the range of 4x10-5-6x10-7 A/m 2 in the same direction. As both ferroelectric and piezoelectric properties of LiTaO 3 films are dependent on film thickness, an optimal energy conversion efficiency was obtained for a thickness of ~3 µm. Furthermore, these devices were tested up to a temperature of 150 °C for voltage generation. Given the need for lead-free piezoelectric materials for environmental applications, these LiTaO 3 cantilevers are very promising for vibrational energy harvester applications especially due to their cost effectiveness, small size, stability at higher temperatures, and repeatable properties which makes them suitable for MEMS devices for industrial applications.