This chapter explores the applications of artificial intelligence (AI) in designing and operating sustainable cloud architecture. Data centers use about 1% of the world’s electricity and are experiencing growing demands due to AI workloads, creating an urgent need for smart solutions that reduce environmental impact. The chapter identifies important sustainability metrics: Power Usage Effectiveness (PUE), Carbon Usage Effectiveness (CUE), and Water Usage Effectiveness (WUE). It also looks at AI-based methods for optimizing resources, such as predictive analytics, reinforcement learning, and carbon-sensitive scheduling. Case studies from the real world show substantial energy savings ranging from 15% to 40%, offering practical insights on how to incorporate sustainability into cloud infrastructure design and operations.