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Recycling spent lithium-ion batteries is integral to today’s low-carbon environmental protection efforts. The concept of direct regeneration, acknowledged for its environmental sustainability, economic viability, and consistent performance of recycled materials, is gaining prominence. This study presents an efficient and nondestructive approach by utilizing an ultrafast microwave technology to directly regenerate spent lithium cobaltate (LCO) cathode materials. In contrast to conventional furnace-based processes, this method significantly reduces the regeneration timeframe. By subjecting the spent LCO mixed with lithium sources to three microwave heating cycles (at approximately 1,350 K), LCO regeneration is achieved, yielding a specific capacity of 140.8 mAh g−1(0.2 C) with a robust cycle stability. With further environmental and economic benefits, the ultrafast microwave technology holds scientific promise for directly regenerating cathode materials, while establishing competitiveness for industrial applications.