The anticorrosive and mechanical properties of carbon nanotubes (CNTs) in epoxy resin (EP) coatings have been improved by the integration of molybdenum disulfide (MoS2) and 3‐aminopropyltrimethoxysilane (APTMS) for surface modification based on CNTs. SEM/EDX, TEM, TGA/XRD, XPS, and XRD techniques were used to characterize the composites for the various formulations, including APTMS/CNTs, CNTs/MoS2, and APTMS/CNTs‐MoS2. By including APTMS/CNTs‐MoS2 composite, the EP coating exhibits improved anticorrosive and mechanical performance, as demonstrated by electrochemical methods and mechanical testing. Superior hydrophobic property of EP‐APTMS/CNTs‐MoS2 is confirmed by its WCA of 167°. Additionally, it was discovered that the EP‐APTMS/CNTs‐MoS2 had a resistance that was significantly larger (17,421 kΩ.cm2) than the plain epoxy (102 kΩ.cm2), and its hardness (1695 MPa), adhesion (19.7 MPa), and tensile (237 MPa) properties all are improved significantly. Therefore, the newly developed EP‐APTMS/CNTs‐MoS2 could act as the vital material for coating AA7475 aluminum alloy used in aerospace applications.