Ti3C2Tx and other types of MXene nanosheets are an exciting new class of 2D materials. However, little has been reported on manipulating the shape of MXene nanosheets. Here, we demonstrate that flat Ti3C2Tx nanosheets encapsulated within spray-dried droplets can be scrolled, bent, and folded into 3D crumpled structures. This morphological change was observed to be reversible upon rehydration.