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The capacitance of MnO2 supercapacitors (SCs) is not high as expected due to its low conductivity of MnO2. The synergistic effects of MnO2 with high theoretical specific capacitance and TiN with high theoretical conductivity can extremely enhance the electrochemical performance of the MnO2-TiN electrode material. In this work, we synthesized different nanostructured and crystalline-structured MnO2 modified TiN nanotube arrays electrode materials by hydrothermal method and explained the formation mechanism of different nanostructured and crystalline-structured MnO2. The influences of MnO2 nanostructures and crystalline-structures on the electrochemical performance has been contrasted and discussed. The specific capacitance of δ-MnO2 nanosheets-TiN nanotube arrays can reach 689.88 F g−1, the highest value among these samples TN-MO-SS, TN-MO-S, TN-MO-SR, TN-MO-RS, and TN-MO-R. The reason is explained based on MnO2 nanostructure and crystalline-structure and electron/ion transport properties. The specific capacitance retention rates are 97.2% and 82.4% of initial capacitance after 100 and 500 cycles, respectively, indicating an excellent charging-discharging cycle stability. [ABSTRACT FROM AUTHOR]