Metal–organic frameworks/zeolitic imidazolate frameworks (MOFs/ZIFs) and their post‐synthesis modified nanostructures, such as oxides, hydroxides, and carbons have generated significant interest for electrocatalytic reactions. In this work, a high and durable oxygen evolution reaction (OER) performance directly from bimetallic Zn100−xCox‐ZIF samples is reported, without carrying out high‐temperature calcination and/or carbonization. ZIFs can be reproducibly and readily synthesized in large scale at ambient conditions. The bimetallic ZIFs show a systematic and gradually improved OER activity with increasing cobalt concentration. A further increase in OER activity is evidenced in ZIF‐67 polyhedrons with controlled particle size of <200 nm among samples of different sizes between 50 nm and 2 μm. Building on this, a significantly enhanced, >50 %, OER activity is obtained with ZIF‐67/carbon black, which shows a low overpotential of approximately 320 mV in 1.0 m KOH electrolyte. Such activity is comparable to or better than numerous MOF/ZIF‐derived electrocatalysts. The optimized ZIF‐67 sample also exhibits increased activity and durability over 24 h, which is attributed to an in situ developed active cobalt oxide/oxyhydroxide related nanophase.