In this paper, the authors report on the use of multilayered carbon nanotubes and graphene films for the fabrication of temperature sensitive resistors. Multiwalled carbon nanotubes- and graphene-based films possess moderate temperature coefficients of resistance and wideband infrared absorption efficiency. This work demonstrates that by incorporating these nanoparticles into a thermally and electrically insulating polymer, polystyrene, the temperature sensitivity significantly improves. Experimental results show temperature coefficients of resistances for these films as high as −0.7%/K. The layers were deposited using a spraying setup without further chemical or thermal treatment. The low cost, simple, and versatile deposition process, in addition to the high temperature coefficients of resistances for these films, makes them suitable alternatives for infrared image sensors as well as many other sensing applications.