Diamond nanoparticle (DN)-coated CNTs were synthesized using a cationic surfactant-assisted sonochemical method. The as-prepared DN coated CNTs were characterized using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). The results show that the DNs were coated on the outer wall surface of CNTs. The DN-coated CNTs were infused in Nylon-6 polymer through a melt extrusion process to form nanocomposite fibers that were tested for their tensile properties. The ultimate tensile strength is found to be 363 MPa for DN/CNTs/Nylon-6 single fibers as compared to 240 MPa for neat Nylon-6 single fibers. These results were also compared with Nylon-6 fibers infused with pristine CNTs and pristine DNs.