Ammonia (NH3) synthesis has been pivotal in various industries, historically relying on the energy-intensive Haber-Bosch process. To address environmental concerns and energy sustainability, researchers have turned to electrochemical methods for NH3 production. The nitrate reduction reaction (NIRR) has emerged as a promising route, bypassing the challenges associated with nitrogen gas (N2) solubility. By converting nitrate (NO3−) to NH3, the process not only tackles water pollution but also offers a sustainable solution. However, the NIRR process is intricate, necessitating efficient electrocatalysts to enhance selectivity and efficiency. Titanium hydride, known for its hydrogen storage capabilities, has shown remarkable performance in electrochemical NH3 synthesis. Through electrochemical hydrogenation reconstruction of titanium fiber paper, a high NH3 yield rate and Faradaic efficiency were achieved, showcasing the potential of titanium hydride as an electrocatalyst for ammonia production. The study elucidated the involvement of lattice hydrogen in the NIRR process, proposing a mechanism that enhances catalytic activity and stability. This finding extends to other metal hydrides, offering a universal design concept for sustainable ammonia synthesis. The research opens new avenues for efficient and eco-friendly NH3 production, emphasizing the importance of innovative electrocatalytic strategies in addressing global energy challenges.