Abstract The popular metal‐ion batteries (MIBs) suffer from environmental and economic issues because of their heavy dependency on nonrenewable metals. Here, we propose a metal‐free ammonium (NH4+)‐based dual‐ion battery with a record‐breaking operation voltage of 2.75 V. The working mechanism of this sustainable battery involves the reversible anion (PF6−) intercalation chemistry in graphite cathode and NH4+ intercalation behavior in PTCDI (3,4,9,10‐perylenetetracarboxylic diimide) anode. This new battery configuration successfully circumvented the reduction susceptibility of NH4+ and the lack of mature NH4+‐rich cathodes for NH4+ ion batteries (AIBs). The customized organic NH4+ electrolyte endows the graphitePTCDI full battery with durable longevity (over 1000 cycles) and a high energy density (200 Wh kg−1). We show that the development of AIBs should be high‐voltage‐oriented while circumventing low operation potential to avoid NH4+ reduction.
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