To improve the chemical and physical surface features of aramid fibers and the bonding quality at the interface, carbon nanotubes, dopamine and silane coupling reagent KH560 were used to modify the surface of aramid fibers. The fiber surface was characterized by FTIR, XPS, SEM and AFM. The single-fiber specific strength, surface roughness, wettability and interfacial shear strength of the modified fiber were quantified. Finally, the uniaxial tensile behaviour of the textile composite laminate with the modified fibers was tested. The experimental results show that: after the grafting of silane coupling reagent as a second modification step, the amount of oxygen-containing groups on the surface of aramid fibers, and the surface roughness, and the ability to impregnate resin are further improved. The single-fiber specific strength, the interfacial shear strength by fiber pull-out tests, and the tensile strength of the laminate are increased by 21.62%, 73.57%, and 51.60%, respectively. This work demonstrates a general surface modification strategy working for diverse types of fibers, synthetic or natural. The present findings help to develop a broad range of high-performance textile composites to address long-term challenges in structural engineering.