“…As established well, sur‐/interface engineering plays a crucial role in enhancing thermal stability and electrochemical behaviors of Ni‐based cathodes for LIBs . Various compounds (Al 2 O 3 , SiO 2 , TiO 2 , ZrO 2 , Li 2 O·2B 2 O 3 , and AlF 3 ) depressing the surface side reactions, and some other materials (Li 3 PO 4 , Li 3 VO 4 , and Li 2 TiO 3 ) improving ionic conductivity, as well as several composites (AlPO 4 , V 2 O 5 , Co 3 (PO 4 ) 2 ) consuming the surface residual lithium have been put forward, and successfully applied to ameliorate the interfacial structural stability of Ni‐based electrodes. Admittedly, all these coating phases to some extent play a constructive role in propelling the practical application of Ni‐based cathodes.…”