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This paper presents an experimental investigation of the bond strength between carbon fiber reinforced polymer (CFRP) and steel substrate by utilizing the pull-off test and scanning electron microscope (SEM) analysis. A series of pull-off experiments was conducted by using three types of CFRP (CFRP sheets and CFRP laminates with/without woven mesh) and two types of epoxy adhesive (ductile and brittle epoxy adhesive) with/without carbon nanotube (CNT) modification. Pull-off samples with CFRP laminates possess higher (about double) bond strength than that of samples with CFRP sheets, due to the good saturation of fibers in the laminates. The steel-CFRP bond with ductile epoxy adhesive (Araldite 2011) is found to have about 16% higher bond strength when compared to that of brittle epoxy (MBrace Saturant), even though the tensile strength of Araldite 2011 is about 40% less than that of MBrace Saturant. Also, it is shown that modified epoxy with CNTs is more efficient than neat epoxy for bonding CFRP to steel at a moderately elevated temperature, and increasing the bond strength about twofold.