A current challenge for the fabrication of functional oxide-based devices is related with the need of environmental and sustainable materials and processes. By considering both lead-free ferroelectrics of potassium sodium niobate (K0.5Na0.5NbO3, KNN) and aqueous-based electrophoretic deposition here we demonstrate that an eco-friendly aqueous solution-based process can be used to produce KNN thick coatings with improved electromechanical performance. KNN thick films on platinum substrates with thickness varying between 10 and 15 μm have a dielectric permittivity of 495, dielectric losses of 0.08 at 1 MHz, and a piezoelectric coefficient d33 of ∼70 pC/N. At TC these films display a relative permittivity of 2166 and loss tangent of 0.11 at 1 MHz. A comparison of the physical properties between these films and their bulk ceramics counterparts demonstrates the impact of the aqueous-based electrophoretic deposition (EPD) technique for the preparation of lead-free ferroelectric thick films. This opens the door to the possible development of high-performance, lead-free piezoelectric thick films by a sustainable low-cost process, expanding the applicability of lead-free piezoelectrics.