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Metal‐oxo clusters have emerged as advanced proton conductors with well‐defined and tunable structures. Nevertheless, the exploitation of metal‐oxo clusters with high and stable proton conductivity over a relatively wide temperature range still remains a great challenge. Herein, three sulfate groups decorated zirconium‐oxo clusters (Zr6, Zr18, and Zr70) as proton conductors are reported, which exhibit...