Sustainable ammonia synthesis, a key focus in electrochemistry, has seen significant advancements with the emergence of Metal‐Organic Frameworks (MOFs). This review provides a comprehensive analysis of the recent strides in MOF‐based materials for green ammonia production, reflecting the urgency to develop eco‐friendly and energy‐efficient chemical commodities. It explores the reaction mechanisms, emphasizing the importance of structure‐performance relationships in MOF optimization and the design of MOF‐based electrocatalysts, including metal node engineering and hybrid materials. The review also highlights in‐situ characterization techniques that are crucial for understanding MOF catalytic activity. It establishes a correlation between MOF features, synthesis methods, and material performance, showcasing their potential in catalysis. Finally, it identifies challenges and future directions for MOFs in green ammonia production, aiming to inspire innovation towards sustainable and economically viable processes.