In this paper, a highly sensitive paper-based humidity sensor is designed and fabricated to overcome the typically low sensitivity and small quality factor of paper-based chipless radio-frequency identification (RFID) humidity sensors. A toroidal inductor-interdigitated electrodes (IDE) capacitor is used as the resonator structure of the new sensor, and the structural parameters of the sensor are optimized using the software of high frequency structure simulator (HFSS) to improve the quality factor. Three paper-based sensor samples were fabricated via screen printing using regular printing paper, Kodak photo paper, and double-sided copper-coated paper as the substrate. In addition, the resonance characteristics, sensitivity, recovery characteristics, stability and other sensor performances were tested. The results show that the sensitivity of the copper-coated-paper-based sensor is significantly better than the two other paper-based sensors. The simulation and test results of the moisture-sensitive characteristics are consistent for graphene oxide (GO) films, which were prepared using the spray method on the surface of the copper-coated-paper-based sensor with mass concentrations of 1 mg/mL, 2 mg/mL, and 5 mg/mL. This indicates that GO films can significantly improve sensor sensitivity when combined with paper-based moisture sensing. Furthermore, the sensitivity increases with increasing GO concentration, the 5 mg/mL GO sensor show a sensitivity of 6.25 MHz/%RH and a range of 60% RH-90% RH. The 1 mg/mL GO humidity sensor shows good recovery characteristics (92.4% recovery). Based on the presence of hydrophilic functional groups in the GO material, a moisture sensing mechanism that GO could improve the sensitivity of the sensor is analyzed.