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[Display omitted] • A general strategy is proposed for the upcycling of residual anodes derived from retired Li-ion batteries into highly valuable electrocatalysts. • The LIB residues are converted into Mn oxide nanoparticles anchored by N and S sites on rGO nanosheets (Mn/NS-rGO). • The binding between Mn and N/S dopants simultaneously optimizes the intermediate adsorption and charge distribution at Mn/rGO interface. • Mn/NS-rGO assembled Al-air battery exhibits an excellent discharge performance under flexible working conditions. Upcycling retired lithium-ion batteries (LIBs) into value-added electrocatalysts represents a promising strategy for tuning the trash into treasure. Herein, an effective approach is reported to convert the LIB anode residues into electrocatalysts that enhance the oxygen reduction reaction (ORR). The residues are utilized for synthesizing reduced graphene oxides (rGO) with Mn nanoparticles anchored by N and S dopants (Mn/NS-rGO). A Pt/C-comparable ORR performance is achieved in alkaline media, with the onset and half-wave potentials of 1.01 and 0.87 V, as well as the excellent durability. Density functional theory (DFT) calculations reveal that Mn sites, coordinating with N and S dopants, simultaneously optimize the intermediate adsorption and charge distribution, which in turn facilitates ORR. The solid-state Al-air batteries are assembled by using Mn/NS-rGO as the cathode catalyst, showing the power density of 103.8 mW cm −2, which successfully charge a cell phone and power LED lights under flexible working conditions. [ABSTRACT FROM AUTHOR]