Surface interaction is extremely important to both fundamental research and practical application. Physisorption can induce shape and structural distortion (i.e., conformational changes) in macromolecular and biomolecular adsorbates, but such phenomena have rarely been observed on adsorbents. Here, it is demonstrated theoretically and experimentally that atomically thin boron nitride (BN) nanosheets as an adsorbent experience conformational changes upon surface adsorption of molecules, increasing adsorption energy and efficiency. The study not only provides new perspectives on the strong adsorption capability of BN nanosheets and many other two-dimensional (2D) nanomaterials but also opens up possibilities for many novel applications. For example, it is demonstrated that BN nanosheets with the same surface area as bulk hexagonal BN particles are more effective in purification and sensing.