The silver paste electrode of piezoelectric (PZT) ceramic discs has been shown to produce a weak interface bond between a bare PZT and its paste coating under a peeling force. In this work, an investigation was conducted to reinforce the bond with a high density array of oriented carbon nanotube nano-electrodes (CNTs-NEA), between a bare PZT ceramic and a metal substrate. The ensuing design and fabrication of a carbon-nanotube-coated piezoelectric disc (CPZT) is presented along with a study of the bondline integrity of a CPZT mounted on a hosting structure. The CPZT has its electrode silver paste coating replaced with a high density array of CNTs-NEA. Mechanical tests were performed to characterize the shear strength of the bondline between CPZT discs and the substrate. The test results were compared with shear strengths of the bondlines made of pure non-conductive adhesive and adhesive with randomly mixed CNTs. The comparison showed the oriented CNT coating on PZTs could significantly enhance the interfacial shear strength. Through the microscopic examination, it was evident that the ratio between the CNT length (Lc) and the bond thickness (H) significantly influenced the bond strength of CPZT discs. Three major interface microstructure types and their corresponding failure modes for specific Lc/H values were identified. The study also showed that failure did not occur along the interface between the PZT ceramic element and the CNT coating.