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The production of metal–organic framework (MOF) nanoplates with well‐defined geometric morphology is remarkable for expanding their applications. Herein, the cobalt‐based MOF nanoplates with hexagonal channels from a layer‐pillared MOF are accomplished, via a molecular scalpel strategy, utilizing monodentate pyridine to replace the bidentate 4,4′‐bipyridine. The morphology can be modified from nanorods to nanoplates with controllable thickness tuned by the amounts of pyridine. Succeeding carbonization treatment transforms the MOF nanoplates into Co particles homogeneously encapsulated in the nitrogen‐doped carbon layers. The prepared catalyst with a unique platelike morphology displays a high half‐wave potential of 0.88 V in oxygen reduction reaction. When used in primary Zn−air batteries, it delivers a high peak power density of 280 mW cm−2. This work clarifies the structure‐morphology‐reactivity connection of MOF nanoplates. [ABSTRACT FROM AUTHOR]