In article number 1903265, Yong‐Mook Kang, Seong‐Ju Hwang, and co‐workers develop an efficient way to improve the electrocatalyst and Li–O2 battery performances of metal oxide via synergistic control of structural disorder and surface bonding nature. The amorphization and iodate anchoring are quite effective in improving electrocatalyst/electrode functionalities of δ‐MnO2 via the alteration of surface bonding character, the stabilization of Mn3+ species, and the enhanced charge transfer of interfaces.