Increasing the temperature variation rate is a useful method for enhancing the response of pyroelectric devices. A three-dimensional ZnO film was fabricated by the aerosol deposition (AD) rapid process using the shadow mask method, which induces lateral temperature gradients on the sidewalls of the responsive element, thereby increasing the temperature variation rate. To enhance the quality of the film and reduce the concentration of defects, the film was further treated by laser annealing, and the integration of a comb-like top electrode enhanced the voltage response and reduced the response time of the resulting ZnO pyroelectric devices.