This paper presents a straightforward method to develop a nanoporous graphene oxide (NGO)-functionalized quartz crystal microbalance (QCM) gas sensor for the detection of trimethylamine (TMA), aiming to form a reliable monitoring mechanism strategy for low-concentration TMA that can still cause serious odor nuisance. The synthesized NGO material was characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy to verify its structure and morphology. Compared with the bare and GO-based QCM sensors, the NGO-based QCM sensor exhibited ultra-high sensitivity (65.23 Hz/μL), excellent linearity (R² = 0.98), high response/recovery capability (3 s/20 s) and excellent repeatability (RSD = 0.02, n = 3) toward TMA with frequency shift and resistance. Furthermore, the selectivity of the proposed NGO-based sensor to TMA was verified by analysis of the dual-signal responses. It is also proved that increasing the conductivity did not improve the resistance signal. This work confirms that the proposed NGO-based sensor with dual signals provides a new avenue for TMA sensing, and the sensor is expected to become a potential candidate for gas detection.