To address the challenge of fabricating thin-film resistors with high stability using conventional materials, a novel chromium-silicon-nickel-molybdenum (Cr-Si-Ni-Mo) alloy thin-film resistor exhibiting a low temperature coefficient of resistance (TCR) is developed in this work, based on the conductive mechanism of thin-film resistors, through the addition of metallic molybdenum (Mo) into conventional nickel-chromium-silicon (Ni-Cr-Si) films. The effects of sputtering power, sputtering time, sputtering pressure, and annealing temperature on the electrical properties of Cr-Si-Ni-Mo thin films are systematically investigated, and the deposition rate of the film layers is evaluated. Experimental results demonstrate that by optimizing sputtering processes and annealing temperature, an optimized Cr-Si-Ni-Mo thin-film resistor is developed using a sputtering power of 300 W, a sputtering time of 210 S, a sputtering pressure of 0.4 Pa, followed by annealing at 300 °C, achieving an exceptional TCR of -5.09 ppm/°C.