The development of efficient electrocatalysts to generate key *NH2 and *CO intermediates is crucial for ambient urea electrosynthesis with nitrate (NO3−) and carbon dioxide (CO2). Here we report a liquid‐phase laser irradiation method to fabricate symbiotic graphitic carbon encapsulated amorphous iron and iron oxide nanoparticles on carbon nanotubes (Fe(a)@C‐Fe3O4/CNTs). Fe(a)@C‐Fe3O4/CNTs exhibits superior electrocatalytic activity toward urea synthesis using NO3− and CO2, affording a urea yield of 1341.3±112.6 μg h−1 mgcat−1 and a faradic efficiency of 16.5±6.1 % at ambient conditions. Both experimental and theoretical results indicate that the formed Fe(a)@C and Fe3O4 on CNTs provide dual active sites for the adsorption and activation of NO3− and CO2, thus generating key *NH2 and *CO intermediates with lower energy barriers for urea formation. This work would be helpful for design and development of high‐efficiency dual‐site electrocatalysts for ambient urea synthesis.

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A schematic representation of MoS2 nanosheet synthesis and its photothermal-triggered drug delivery application.