Interface bonding conditions between concrete and steel materials play key roles in ensuring the composite effect and load-carrying capacity of concrete-steel composite structures such as concrete-filled steel tube (CFST) members in practice. A method using both surface wave and electromechanical impedance (EMI) measurement for detecting the existence and the location of inaccessible interface debonding defects between the concrete core and steel tube in CFST members using piezoelectric lead zirconate titanate (PZT) patches as actuators and sensors is proposed. A rectangular CFST specimen with two artificially mimicked interface debonding defects was experimentally verified using PZT patches as the actuator and sensor. By comparing the surface wave measurement of PZT sensors at different surface wave travelling paths under both a continuous sinusoidal signal and a 10-period sinusoidal windowed signal, three potential interface debonding defects are quickly identified. Furthermore, the accurate locations of the three detected potential interface debonding defects are determined with the help of EMI measurements from a number of additional PZT sensors around the three potential interface debonding defects. Finally, the accuracy of the proposed interface debonding detection method is verified with a destructive observation by removing the local steel tube at the three detected interface debonding locations. The observation results show that the three detected interface debonding defects are two mimicked interface debonding defects, and an unexpected debonding defect occurred spontaneously due to concrete shrinkage in the past one and a half years before conducting the test. Results in this study indicate that the proposed method can be an efficient and accurate approach for the detection of unknown interface debonding defects in existing CFST members.