Two-dimensional (2D) non-layered materials, along with their unique surface properties, offer intriguing prospects for sensing applications. Introducing mechanical degrees of freedom is expected to enrich the sensing performances of 2D non-layered devices, such as high frequency, high tunability, and large dynamic range, which could lead to new types of high performance nanosensors. Here, we demonstrate 2D non-layered nanomechanical resonant sensors based on β-In2S3, where the devices exhibit robust nanomechanical vibrations up to the very high frequency (VHF) band. We show that such device can operate as pressure sensor with broad range (from 10−3 Torr to atmospheric pressure), high linearity (with a nonlinearity factor as low as 0.0071), and fast response (with an intrinsic response time less than 1 μs). We further unveil the frequency scaling law in these β-In2S3 nanomechanical sensors and successfully extract both the Young's modulus and pretension for the crystal. Our work paves the way towards future wafer-scale design and integrated sensors based on 2D non-layered materials.