Atmospheric water harvesting (AWH) offers a promising solution to the escalating global water crises. Among its variants, sorption-based AWH (SAWH) is particularly notable for its adaptability across a range of climates. In this Review, we delve into the complexities of sorbent materials, discussing foundational sorption dynamics, advances in material design, and the strategies for scale-up processing. The analysis extends to system engineering, particularly the optimization of thermal and mass-transfer processes essential for effective operation across different scenarios. By synthesizing insights from materials, systems, and climate, we tackle the challenges of energy management, operational strategies, and multifunctional applications. We outline a strategic roadmap for the practical implementation of SAWH technologies, underscoring their potential to significantly enhance sustainable water solutions globally.