Upcycling Strategy for Mixed Spent Batteries to Enable NMC622 & Graphite Full Batteries

The rapid growth of lithium‐ion batteries is intensifying pressure on critical‐material supply chains while generating increasing volumes of complex battery waste. However, existing recycling technologies struggle to process mixed feedstocks efficiently and often recover products with limited added value. Here, we advance beyond cathode‐focused hydrometallurgical recycling by integrating composition‐adjustable cathode resynthesis with the purification and surface modification of co‐recovered graphite, followed by full‐pouch‐cell validation and unified process‐level assessment. Mixed low‐nickel cathodes are upgraded to high‐performance LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) with improved lithium‐ion transport and cycling stability. Meanwhile, a closed‐loop graphite upcycling process produces battery‐grade anodes with enhanced interfacial kinetics and durability. Full pouch cells assembled entirely from the upcycled materials exhibit fewer side reactions and approximately twice the cycle life of cells using commercial counterparts, retaining 70% of their capacity after 2590 cycles. Techno‐economic and life‐cycle analyses further indicate >95% recycled‐material utilization, 22.9% higher profitability, and reductions of 27.0% in greenhouse‐gas emissions and 29.4% in energy consumption relative to the reference recycling route. These findings establish mixed battery waste as a viable feedstock for producing high‐value battery materials and demonstrate a pathway from conventional resource recovery toward value‐added remanufacturing for circular, resilient, and low‐carbon battery supply chains.