Transition‐metal selenides based materials have recently aroused an increasing consideration in the field of energy reservation and conversion owing to their good electrochemical performance and low synthetic cost. Herein, multi‐walled carbon nanotubes supported binary nickel cobalt selenide composite (Ni−Co−Se/CNT) was prepared by a one‐pot‐hydrothermal method using hydrazine ions that enables the selenium to diffuse and react with the Ni‐and Co‐cations to form Ni−Co−Se with a stable nanostructure onto the outer walls of the CNT platforms due to the coordination interaction between the metallic cations and surface oxygen‐containing group of the conductive scaffolds. The electrochemical performances for urea oxidation reaction (UOR) are accessed in an alkaline medium by cyclic voltammetry (CV), chronopotentiometry (CA), and electrochemical impedancespectroscopy (EIS) tests. The as‐prepared Ni−Co−Se/CNT hybrid presents an excellent electrocatalytic activity in terms of current density and onset potential due to synergistic effects of tubular CNT scaffolds, additional Co active sites, and electrochemically active NiOOH layer. The CNTs support markedly enhanced the electrocatalytic properties by providing a rapid mass transport for UOR because of their porous network architectures with a robust adhesion to the Ni−Co−Se nanocrystals. Thus, the synthetic methodology synthetic methodology adopted here is entirely effective for constructing various metal selenide compounds in future.