The trace-level detection of harmful NO2 gas at room-temperature is very important for environmental protection and public health. This paper reports the resonant-gravimetric detection of ppb-level NO2 at room-temperature using two-dimensional porous TiO2 nanosheets (PTNSs) as highly active sensing materials. They are synthesized by a facile high-temperature calcination approach based on a graphene oxide self-sacrificial template. The PTNS sample prepared at 500 °C (TiO2-500 °C) show an anatase structure, while the sample prepared at 800 °C (TiO2-800 °C) contains an impurity rutile phase. By loading pure anatase PTNSs onto resonant microcantilevers, the sensors exhibit high sensitivity to NO2 gas with a limit of detection as low as 15 ppb. Compared with the TiO2-800 °C sample, the much higher sensitivity of the TiO2-500 °C sample can be attributed to the bigger adsorption enthalpy (-ΔH°) of pure anatase TiO2 to NO2 gas molecules (21.7 and 57.8 kJ mol-1, respectively). Density functional theory calculations further demonstrate that the existence of the rutile impurity phase in the TiO2-800 °C sample results in its significantly decreased adsorption activity to NO2. This work approves the great application potential of anatase PTNSs for the highly sensitive resonant-gravimetric detection of NO2 gas at room-temperature.