Abstract The resonance frequency of ultra-thin layered nanomaterials changes nonlinearly with the tension induced by the pressure from the surrounding gas. Although the dynamics of pressurized nanomaterial membranes have been extensively explored, recent experimental observations show significant deviations from analytical predictions. Here, we present a multi-mode continuum model that captures the nonlinear pressure-frequency response of pre-tensioned membranes undergoing large deflections. We validate the model using experiments conducted on polysilicon nanodrums excited opto-thermally and subjected to pressure changes in the surrounding medium. We demonstrate that considering the effect of pressure on the nanodrum tension is not sufficient for determining the resonance frequencies. In fact, it is essential to also account for the change in the membrane’s shape in the pressurized configuration, the mid-plane stretching, and the contributions of higher modes to the mode shapes. Finally, we show how the presented high-frequency mechanical characterization method can serve as a fast and contactless method for determining Young’s modulus of ultra-thin membranes.