The use of electrochemical impedance spectroscopy based sensor technology for NDE of bond degradation between external CFRP reinforcement and concrete is examined. Copper tape on the surface of the CFRP sheet, stainless steel wire embedded in the concrete, and reinforcing bars were used as the sensing elements. Laboratory experiments were designed to test the capability of the sensors to detect the debonding of the CFRP from the concrete. The CFRP sheet was debonded from the concrete and impedance measurements were taken between various pairs of electrodes at various interfacial crack lengths. The dependence of the impedance spectra, and of the parameters obtained from equivalent circuit analysis, on the interfacial crack length was studied. Capacitance parameters in the equivalent circuit correlated strongly with the interfacial crack length. The capacitance can be used to assess the global state of the bond between CFRP sheets and concrete. Impedance measurements taken between embedded wire sensors can be used to detect the location of debonded regions.