Binder-less, self-standing, disposable, and costeffective sensing probes are crucial for the development of nextgeneration nonenzymatic urea sensors (NEUSs). In the present study, three-dimensional (3D) coral-like NiFe-based layered double hydroxide (NF-LDH) microstructures were grown over the naturally inherited porous microchannels of nitrogen-doped carbonized wood (NCW). The microstructural details and chemical composition of the fabricated electrodes were examined by microscopic and spectral methods. The formation of novel 3D coral-like microarchitectures with uniformly enveloped nanoflakes was evidenced from the scanning electron microscopy measurements. Interestingly, NF-LDH exhibited a voltammetric response for urea due to the unique 3D architecture and synergistic influence between catalytically active Ni 3+ sites and doped Fe 3+ centers. Here, NCW serves as a catalyst-docking platform and electronconducting medium. Such direct anchoring of catalytically active structures on conductive scaffolds eliminates the electron transfer resistance provoked by stereotypical insulating binders. Furthermore, the growth of the NF-LDH catalyst on NCW was varied with respect to the mole ratio of Ni 3+ and Fe 3+ . Among the different mole ratios, the NF-LDH catalyst modified with Ni/Fe-0.75:0.25 showed the best sensing performance toward urea with a sensitivity of 53 μA mM −1 cm −2 , a wide linear range from 0.5 to 8 mM, and a limit of detection of 0.114 mM (S/N = 3) in addition to exceptional stability and reproducibility.