The severe energy crisis and environmental issues have led to an increase in research on the development of sustainable energy. Atomically thin 2D multinary nanosheets with tunable components show advantages for producing sustainable energy via photo, electrocatalysis processes. Here, recent progress of atomically thin 2D multinary nanosheets from the design, synthesis, tuning, and sustainable energy production via photo, electrocatalysis processes is summarized. The regulating strategies such as alloying, doping, vacancy engineering, pores construction, surface modification, and heterojunction are summarized, focusing on how to optimize the catalytic performance of atomically thin 2D multinary nanosheets. In addition, advancements in versatile energy‐related photo, electrocatalytic applications in the areas of oxygen evolution, oxygen reduction, hydrogen evolution, CO2 reduction, and nitrogen fixation are discussed. Finally, existing challenges and future research directions in this promising field are presented.