A process of making an electrochromic or an electrolytic film by Ultrasonic Spray Pyrolysis (USP) deposition on a substrate comprising: mixing a surfactant to an aqueous precursor solution comprising an electrochromic component or an electrolytic component to provide a spray solution; introducing the spray solution into an ultrasonic spray deposition nozzle at a constant flow rate between 0.1 mL/min and 2 mL/min and applying an ultrasonic frequency between 80 and 120 kHz to generate atomized droplets of the precursor solution; entraining the atomized droplets with a controlled jet of air as gas carrier at a pressure between 0.50 to 2.0 psi, onto a pre-heated substrate at a temperature of 200 to 450° C.; thermally converting the atomized droplets when depositing onto the pre-heated substrate to generate an electrochromic or an electrolytic film.