Electrochemical oxidation of urea (UOR) is critical in the removal of urea from wastewater and energy conservation and storage. Nickel-based catalysts are widely used for urea-ORR, but in all cases, the nickel must be hybridized with carbon materials to improve its conductivity. In this manuscript, we demonstrate the synthesis of a nickel-decorated carbon nanotube (Ni-NCNT) by simple microwave pyrolysis of Dabco (1,4-diazabicyclo[2.2.2]octane)-based coordination polymer frameworks (CPF). The surface structure, morphology and chemical composition of Ni-NCNT were characterized by Raman spectrum, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy (EDS) analysis. SEM studies showed micrometer-long bamboo-shaped CNTs with nickel nanoparticles anchored to the walls and inside the nanotubes. A structural study by TEM and Raman spectra showed that carbon nanotubes are rich in defects due to the presence of nitrogen, and this was confirmed by energy-dispersive X-ray spectroscopy (EDS) maps. When applied as electrocatalysts in urea oxidation reactions (UOR), our newly developed Ni-NCNT shows excellent electrocatalytic activity and stability, making it a versatile catalyst in energy generation and mitigating water contamination.