The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications. Electroreduction of carbon dioxide (CO) directly into such high value-added chemicals can help us achieve a renewable C cycle. Such electrochemical reduction typically suffers from low faradaic efficiencies (FEs) and generates a mixture of products due to the complexity of controlling the reaction selectivity. This perspective summarizes recent advances in the mechanistic understanding of CO reduction reaction pathways toward liquid products and the state-of-the-art catalytic materials for conversion of CO to liquid C (e.g., formic acid, methanol) and C products (e.g., acetic acid, ethanol, -propanol). Many liquid fuels are being produced with FEs between 80% and 100%. We discuss the use of structure-binding energy relationships, computational screening, and machine learning to identify promising candidates for experimental validation. Finally, we classify strategies for controlling catalyst selectivity and summarize breakthroughs, prospects, and challenges in electrocatalytic CO reduction to guide future developments.