The combination of high-performance steel with aluminum or aluminum alloys shows a wide range of application in high technologies field like aerospace, smart materials, etc. The problem in using of adhesive bonding technology for these substrates is the weak mechanical occlusion between steel/aluminum and common coatings. In this study, different methods of treatment of carbon fiber were employed to enhance the adhesion strength in steel-epoxy resin filled with carbon fiber-aluminum triplex. The treatment of carbon fibers with 3-glicidyloxypropyl-trimetoxysilane after their oxidation in 65 wt.% nitric acid leads to the additives which improve the adhesion strength of epoxy resins at 15 wt.% contain on 67.5% in comparison with neat epoxy up to 20 MPa. This result can be explained by the change of failure mechanism from “cohesive’ to “adhesive” that leads to an increase of adhesion strength to steel and aluminum. The SEM study shown that 60–80 nm thick two-layer interphase formed between carbon fiber and epoxy matrix. The mechanical strength of this interphase governs the mechanical and adhesion performance of steel-epoxy resin-aluminum triplex. Taking into account the mechanical properties and adhesive strength of these composites, it emerges as a potential candidate for advanced materials.