Electrochemistry could play a critical role in the transition to a more sustainable society by enabling the carbon-neutral production and use of various chemicals as well as efficient use of renewable energy resources. A prerequisite for the practical application of various electrochemical energy conversion and storage technologies is the development of efficient and robust electrocatalysts. Recently, molecularly designed heterogeneous catalysts have drawn great attention because they combine the advantages of both heterogeneous solid and homogeneous molecular catalysts. In particular, recently emerged metal-phenolic networks (MPNs) show promise as electrocatalysts for various electrochemical reactions owing to their unique features. They can be easily synthesized under mild conditions, making them eco-friendly, form uniform and conformal thin films on various kinds of substrates, accommodate various metal ions in a single-atom manner, and have excellent charge-transfer ability. In this minireview, we summarize the development of various MPN-based electrocatalysts for diverse electrochemical reactions, such as the hydrogen evolution reaction, the oxygen evolution reaction, the CO2 reduction reaction, and the N2 reduction reaction. We believe that this article provides insight into molecularly designable heterogeneous electrocatalysts based on MPNs and guidelines for broadening the applications of MPNs as electrocatalysts.