Realizing confined Li2O2 growth and enhanced decomposition kinetics is still a challenge for lithium–oxygen (Li–O2) batteries, which influences its electrochemical performances. Herein, a three‐dimensional (3D) porous sandwich cathode architecture constructed through the self‐assembly of the in situ growing Fe2O3 nanorods on graphitic carbon nitride nanosheets (CNS) together with carbon nanotubes (CNTs) (Fe2O3@CNS‐CNTs) is presented. The formation of Fe–N structure can offer the active sites for the oxygen reduction reaction (ORR) and Fe2O3 nanorods provide the nucleation sites for the growth of Li2O2. Due to the 3D sandwich structure, the Li2O2 nanosheets can be deposited in the inner space of the 3D structure with an embedded mode, which confines the size and distribution of Li2O2. This work offers more possibilities for the realization of the controllable Li2O2 deposition, holding great promise in enlightening the hybrid cathode design for Li–O2 batteries.

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