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The proper handling of end-of-life (EOL) lithium-ion batteries (LIBs) has become an urgent and challenging issue with the surging use of LIBs, in which recovering high-value cathodes not only relieves the pressure on the raw material supply chain but also minimizes environmental pollution. Beyond direct recycling of spent cathodes to their pristine states, the direct upcycling of spent cathodes to the next-generation cathodes is of great significance to maximize the value of spent materials and to sustain the fast development of LIBs. Herein, a "reciprocal ternary molten salts" (RTMS) system was developed to directly upcycle spent NMC 111 to Ni-rich NMCs by simultaneously realizing the addition of Ni and the relithiation of Li in spent NMC 111. After RTMS flux upcycling, the obtained Ni-rich NMCs exhibited an α-NaFeO 2 -type layered structure, restored Li content, and excellent performance, which is very similar to that of the pristine NMC 622., Competing Interests: The authors declare no competing interests., (© 2022 The Author(s).)