Two-dimensional (2D) nanomaterials have been explored for numerous promising applications benefiting from their distinct chemical and physical properties. When 2D nanomaterials meet with the idea of learning from nature, a vaster world expands. In article number 1902806, Ziqi Sun and co-workers introduce the topic of “bioinspired 2D nanomaterials”, along with the current progress, challenges, and opportunities for their applications in sustainable energy and environmental technologies.