Structural electrode materials that integrate high mechanical strength and high electrochemical performances are attractive as they are indispensable for building lightweight, flexible electronics. [1][2][3] These materials should be able to withstand extreme mechanical stress and deformations while maintaining high charge storage properties, and thereby decrease the electrochemically inactive weight and volume for packaging of devices, especially in limited spaces. [1] Most conventional electrode materials, however, fail to meet both requirements. [4] Some of reported strategies involved using carbon fiber-reinforced composites [5,6] or graphene-based materials [1] as structural electrodes to deliver mechanical strength. These materials, however, fall short on the electrochemi cal energy storage capacitance. Alternatively, metal oxides [7] or conducting polymers [8] can be incorporated to boost the capacitance of the graphene-based materials. The problem is the weak interactions between different components, which results in low mecha nical stability of the final composites. [7,9] Therefore, there is a crucial need for the development of new-generation structural energy storage nanocomposites, which monolithically integrate excellent mechanical properties, high electronic and ionic conductivities, and high charge storage capabilities. A balance should also exist between these properties without substantially sacrificing one property over the other. [1] The family of two-dimensional (2D) metal carbides and nitrides, collectively known as MXene, are interesting materials for building high-performance supercapacitors. [10][11][12][13][14][15][16] MXenes have a general formula of M n+1 X n T x , where M is an early transition metal such as Ti, X is carbon or nitrogen, and T x indicates the presence of different functional groups (O, OH, and F) on the surface of metal layers, a result of aqueous exfoliation synthesis of MXenes. [10,17,18] Ti 3 C 2 T x MXene has been widely reported as a high-performance electrode material either in its pristine form or in hybrids with other guest materials such as poly(vinyl alcohol) (PVA), [18] polypyrrole, [19,20] and polyaniline, [21] as well as in hybridization with other carbon materials such as graphene, [22] carbon nanotubes, [23][24][25] and carbon nanofibers. [26] Most of the MXene hybrid nanocomposites, however, have only shown improvement in either capacitance or mechanical properties while sacrificing one property over the other, and they lack the required mechanical integrityThe family of two-dimensional (2D) metal carbides and nitrides, known as MXenes, are among the most promising electrode materials for supercapacitors thanks to their high metal-like electrical conductivity and surface-functional-group-enabled pseudocapacitance. A major drawback of these materials is, however, the low mechanical strength, which prevents their applications in lightweight, flexible electronics. A strategy of assembling freestanding and mechanically robust MXene (Ti 3 C 2 T x ) nanoco...