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Generation of hydrogen fuel via electrochemical water splitting powered by sustainable energy, such as wind or solar energy, is an attractive path toward the future renewable energy landscape. However, current water electrolysis requires desalinated water resources, eventually leading to energy costs and water scarcity. The development of cost‐effective electrocatalysts capable of splitting saline water feeds directly can be an evident solution. Herein, a surface reconstructed nickel‐iron layered double hydroxide (NF‐LDH) is reported as an exceptionally active and durable bifunctional electrocatalyst for saline water splitting without chloride corrosion. The surface reconstructed NF‐LDH consists of Ni3Fe alloy phase interconnected in a 2D network in which an ultrathin (≈2 nm) and low‐crystalline NiFe (oxy)hydroxide phase are formed on the surface. The NiFe (oxy)hydroxide phase draws large anodic current densities, satisfying the level of practical application, while the Ni3Fe alloy phase is simultaneously responsible for the high catalytic activity for cathodic reactions and superior corrosion resistance. The surface reconstructed NF‐LDH electrode can be easily fabricated in a large electrode area (up to 25 cm2) and can successfully produce hydrogen fuels from saline water powered by the laboratory‐made low‐intensity photovoltaic cell. [ABSTRACT FROM AUTHOR]