LAUSR

Open framework materials (OFMs), such as metal‐organic frameworks and covalent organic frameworks have emerged as promising electrocatalysts to address the global energy crisis and environmental problems. Powdered non‐film forms, that is, bulk OFMs exhibit excellent catalytic activities toward electrocatalytic carbon dioxide reduction, water splitting, and the oxygen reduction reaction. However, electrode preparation using bulk solids suffers from a range of oft‐encountered difficulties, primarily limited by challenges in controlling their thickness, roughness, and particle sizes, despite early performance promises. Targeting energy sustainability, it is a matter of growing interest to directly integrate OFMs in the form of thin films onto conductive substrates. In essence, this leads to electrocatalysts with controlled features: thickness, roughness, and particle sizes. Thus far, there are only a handful of OFM thin films developed for electrocatalysis. Exploration of these understudied OFM thin films to serve electrocatalysis still lies at its infancy. This review will cover the key discoveries of OFM thin films as electrocatalysts and will critically examine the strengths, challenges, and future goals in exploring bespoke OFM thin films for electrocatalysis, under conditions that mimic real‐world applications.