The manipulation of interactions between light and matter plays a crucial role in the evolution of organisms and a better life for humans. As a result of natural selection, precise light-regulatory systems of biology have been engineered that provide many powerful and promising bioinspired strategies. As the "king of disguise", cephalopods, which can perfectly control the propagation of light and thus achieve excellent surroundingmatching via their delicate skin structure, have made themselves an exciting source of inspiration for developing optical and thermal regulation nanomaterials. This review presents cuttingedge advancements in cephalopod-inspired optical and thermal regulation nanomaterials, highlighting the key milestones and breakthroughs achieved thus far. We begin with the underlying mechanisms of the adaptive color-changing ability of cephalopods, as well as their special hierarchical skin structure. Then, different types of bioinspired nanomaterials and devices are comprehensively summarized. Furthermore, some advanced and emerging applications of these nanomaterials and devices, including camouflage, thermal management, pixelation, medical health, sensing and wireless communication, are addressed. Finally, some remaining but significant challenges and potential directions for future work are discussed. We anticipate that this comprehensive review will promote the further development of cephalopod-inspired nanomaterials for optical and thermal regulation and trigger ideas for bioinspired design of nanomaterials in multidisciplinary applications.