<p>In this study, we developed a nanocomposite of Ni/Zn/Al-layered double hydroxide (LDH) and metal–organic frameworks (MOFs) through the electrochemical deposition of the Ni/Al LDH at the surface of the carbon ceramic electrode (CCE) and chemical in situ growth of Ni/Zn/Al LDH-MOF nanocomposite under mild conditions. The Ni/Zn/Al LDH-MOF nanocomposite modified CCE was analyzed using a range of instrumental methods. Then, the Ni/Zn/Al LDH-MOFs/CCE was employed for the electrocatalytic oxidation of methanol in alkaline solution. The Ni/Zn/Al LDH-MOFs/CCE shows enhanced electrocatalytic activity in 0.1&#xa0;M sodium hydroxide toward the oxidation of methanol, with anodic peak current density proportional to methanol concentration. In continuation of electrochemical studies, the electron transfer coefficient (<i>α</i>) and the catalytic rate constant (<i>k</i>_cat) for the methanol oxidation reaction at the Ni/Zn/Al LDH-MOF/CCE were measured: <i>α</i> = 0.35 and <i>k</i>_cat = 6.77 × 10⁴ cm³&#xa0;mol⁻¹&#xa0;s⁻¹. The pseudo steady-state polarization method was employed to investigate the electrocatalytic oxidation of methanol at the Ni/Zn/Al LDH-MOFs/CCE, as well as to determine some electrooxidation reaction parameters. The obtained values include the following: <i>k</i>₂Г^* = 1.87 × 10⁻⁹&#xa0;cm&#xa0;s⁻¹ and the ratio of <i>k</i>⁰₋₁/<i>k</i>⁰₁ = 1.8 × 10⁷. These findings indicated that the incorporation of the Zn ions and MOFs into the Ni/Al LDH and the construction of the nanocomposite significantly enhanced the electrocatalytic performance of the resulting electrocatalyst, paving the way for the development of a highly efficient anodic material for direct methanol fuel cell applications.</p>