Supercapacitors possessing multiple functions other than storing energy, such as bearing mechanical loads, are a promising technology for a wide range of applications. However, achieving both energy storage efficiency and mechanical strength/stiffness requires structurally strong electrolytes and high-capacitance electrodes. Herein, we report a novel method of synthesizing a high-mass loading of MnO 2 on carbon nanotube (CNT) mats to create nanocomposite electrodes of high capacitance and mechanical properties. With CNTs acting as structural reinforcement for the pseudocapacitive MnO 2 matrix, the resulting nanocomposite electrodes exhibited an ultrahigh areal capacitance of 2579 mF/cm2 at a current density of 1 mA/cm2 and excellent mechanical properties. These electrodes were then used to fabricate flexible and mechanically strong structural supercapacitors by infusing with a PVA gel electrolyte and a PEGDGE solid electrolyte, respectively. The resulting flexible supercapacitors yielded a high areal capacitance of 947 mF/cm2 while the structural supercapacitors gave a high tensile modulus of 6.1 GPa. These results demonstrated that the hierarchical MnO 2 /CNT electrodes could provide both excellent energy storage capability and structural stiffness and strength, expanding their applications beyond mono-functional supercapacitors. [Display omitted] [ABSTRACT FROM AUTHOR]