The design of smart coatings for corrosion protection aims has become one of the most interesting hotspots for contemporary corrosion researchers. For this purpose, scientists mostly grabbed on the utilization of carriers with control-release capability, and carbonaceous materials are the most well-known celebrities among all. In this work, the multi-walled carbon nanotube (CNT) surface was decorated with ZIF67 crystals, and then MoO42− ions (Mo) were loaded into the constructed nano-carrier. Eventually, the synthesized particles' were covered by (3-Aminopropyl) triethoxysilane (APTES) amino silane for better dispersion in the silane matrix. The silanized and un-modified nano-hybrids were precisely explored by different characteristic methods to prove their successful synthesis. Also, the inductively coupled plasma (ICP) measurements demonstrated around 49 ppm, 18 ppm, and 0.02 ppm Co ions in the acidic, neutral, and alkaline conditions, respectively. The Electrochemical Impedance Spectroscopy (EIS) and polarization records in the solution phase revealed that CNT-ZIF67-Mo nano-hybrids successfully declined the corrosion rate of metal up to 91% and 84%, respectively. Thereupon, to design a self-healable anti-corrosion system, CNT-ZIF67-Mo particles at 0.15 wt% were incorporated into the silane-based hybrid coating. The EIS explorations carried out on the scratched composites proved that the total resistance was tripled and self-healing activity with a 69% index was visualized after the inclusion of APTES/CNT-ZIF67-Mo nanoparticles. Also, the EIS investigations over the intact composites declared that the silane coating resistance was increased from 23156 Ω.cm2 to 200169 Ω.cm2 and water uptake was around 73% upon the incorporation of APTES/CNT-ZIF67-Mo nanoparticles.