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Sodium borohydride (NaBH4) has earned recognition as a promising hydrogen carrier, attributed to its exceptional hydrogen storage capacity, boasting a high theoretical storage capacity of 10.8 wt %. Nonetheless, the utilization of traditional pyrolysis and hydrolysis methods still presents a formidable challenge in achieving controlled hydrogen generation especially under ambient conditions. In this work, we report an innovative electrochemical strategy for production H2 by coupling NaBH4 electrooxidation reaction (BOR) at anode in alkaline media with hydrogen evolution reaction (HER) at cathode in acidic media. To implement this, we have developed a bifunctional electrocatalyst denoted as Pd‐Mo2C@CNTs, wherein Pd nanoparticles are grown in situ on Mo2C embedded within N‐doped carbon nanotubes. This electrocatalyst demonstrates exceptional performance in catalyzing both alkaline BOR and acidic HER. We have developed a hybrid acid/alkali cell, utilizing Pd/Mo2C@CNTs as the anode and cathode electrocatalysts. This configuration showcases remarkable capabilities for self‐sustained, precise, and uninterrupted indirect release of H2 stored in NaBH4, even at high current densities of 100 mA cm−2 with a Faraday efficiency approaching 100 %. Additionally, this electrochemical device exhibits significant promise as a fuel cell, with the ability to deliver a maximum power density of 20 mW cm−2. [ABSTRACT FROM AUTHOR]