Here we demonstrate through experiment and simulation the polymer-assisted dispersion of inorganic 2D layered nanomaterials such as boron nitride nanosheets (BNNSs), molybdenum disulfide nanosheets (MoS2), and tungsten disulfide nanosheets (WS2), and we show that spray drying can be used to alter such nanosheets into a crumpled morphology. Our data indicate that polyvinylpyrrolidone (PVP) can act as a dispersant for the inorganic 2D layered nanomaterials in water and a range of organic solvents; the effectiveness of our dispersion process was characterized by UV-vis spectroscopy, microscopy and dynamic light scattering. Molecular dynamics simulations confirm that PVP readily physisorbs to BNNS surfaces. Collectively, these results indicate that PVP acts as a general dispersant for nanosheets. Finally, a rapid spray drying technique was utilized to convert these 2D dispersed nanosheets into 3D crumpled nanosheets; this is the first report of 3D crumpled inorganic nanosheets of any kind. Electron microscopy images confirm that the crumpled nanosheets (1-2 μm in diameter) show a distinctive morphology with dimples on the surface as opposed to a wrinkled, compressed surface, which matches earlier simulation results. These results demonstrate the possibility of scalable production of inorganic nanosheets with tailored morphology.