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In a previous study, the present group designed and fabricated ZnO thin-film pyroelectric sensors with four different upper electrode configurations, namely rectangular, criss-cross, target and web. However, the voltage response of the proposed devices was not formally analyzed. Accordingly, the present study commences by performing an experimental investigation to determine the voltage-temperature transfer function for one of the four electrode configurations (i.e., rectangular). An optimization algorithm based on the simplified conjugate gradient method (SCGM) and COMSOL finite-element analysis software is then applied to establish the optimal geometry parameters of each of the four upper electrode configurations. It is shown that the optimized electrode designs improve the temperature variation rate of the four sensors by a minimum of 15%. As a result, the responsivity of the proposed devices is significantly improved.