Plasma nanocoating of allylamine were deposited on the surfaces of multi-walled carbon nanotubes (MWCNTs) to provide desirable functionalities and thus to tailor the surface characteristics of MWCNTs for improved dispersion and interfacial adhesion in epoxy matrices. Plasma nanocoated MWCNTs were characterized using scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM), surface contact angle, and pH change measurements. Mechanical testing results showed that epoxy reinforced with 1.0 wt % plasma coated MWCNTs increased the tensile strength by 54% as compared with the pure epoxy control, while epoxy reinforced with untreated MWCNTs have lower tensile strength than the pure epoxy control. Optical and electron microscopic images show enhanced dispersion of plasma coated MWCNTs in epoxy compared to untreated MWCNTs. Plasma nanocoatings from allylamine on MWCNTs could significantly enhance their dispersion and interfacial adhesion in epoxy matrices. Simulation results based on the shear-lag model derived from micromechanics also confirmed that plasma nanocoating on MWCNTs significantly improved the epoxy/fillers interface bonding and as a result the increased composite strength.