The ever‐increasing importance of critical metals (CMs) in modern society underscores their resource security and circularity. Waste‐printed circuit boards (WPCBs) are particularly attractive reservoirs of CMs due to their gamut CM embedding and ubiquitous presence. However, the recovery of most CMs is out of reach from current metal‐centric recycling industries, resulting in a flood loss of refined CMs. Here, 41 types of such spent CMs are identified. To deliver a higher level of CM sustainability, this work provides an insightful overview of paradigm‐shifting pathways for CM recovery from WPCBs that have been developed in recent years. As a crucial starting entropy‐decreasing step, various strategies of metal enrichment are compared, and the deployment of artificial intelligence (AI) and hyperspectral sensing is highlighted. Then, tailored metal recycling schemes are presented for the platinum group, rare earth, and refractory metals, with emphasis on greener metallurgical methods contributing to transforming CMs into marketable products. In addition, due to the vital nexus of CMs between the environment and energy sectors, the upcycling of CMs into electro‐/photo‐chemical catalysts for green fuel synthesis is proposed to extend the recycling chain. Finally, the challenges and outlook on this all‐round upgrading of WPCB recycling are outlined.