Abstract The electrocatalytic reduction reaction of carbon dioxide (CO 2 RR) has gained significant attention as a promising approach to mitigate carbon dioxide emissions and generate valuable chemicals and fuels. However, the practical application of CO 2 RR has been hindered by the lack of efficient and selective electrocatalysts, particularly to produce multi‐carbon (C 2+ ) products. Nature serves as an ideal source of inspiration for the development of CO 2 RR electrocatalysts, as biological organisms can efficiently catalyze the same reaction and possess robust structures that are inherently scaling. In this review, recent advances in the nature‐inspired design of electrocatalysts for CO 2 RR to C 2+ products are summarized and categorized based on their inspiration source, including the coordination sphere of metalloenzymes and the cascade reactions within the enzyme, as well as the local environment. The importance of understanding the fundamental mechanisms and the different contexts between nature and technological application in the design process is highlighted, with the aim to improve the nature‐inspired design of electrocatalysts for CO 2 RR to C 2+ products.