We have investigated the temperature dependence of the piezoelectric coefficients and infrared sensor performance of spin-coated thin films of polyundecylurea (PUA11). The piezoelectric coefficients of the PUA11 films remained constant at temperatures above 180 °C and these films demonstrated thermal resistance superior to those of poly(vinylidene fluoride/trifluoroethylene) [P(VDF/TrFE)] films. The infrared sensor performance of the PUA11 films was measured after annealing at 125 °C for 500 h and was found to have retained 84% of its preannealing level. The thermal stability of the PUA11 films was higher than that of the P(VDF/TrFE) films; moreover, PUA11 is also expected to have superior electrothermal stability.