of the promising candidates for energy storage due to the high power density, environmental friendliness, remarkable charge/discharge capability, long cycling life, and safety. [4,5] Processing nanomaterials into freestanding films with high conductivity and good mechanical stability is of great significance for supercapacitors. To choose appropriate nanomaterials for high-performance supercapacitors, remarkable surface properties, inherent high strength and electrical conductivity must be considered. [6,7] In the search for alternatives that provide all these characteristics, MXene, a recently discovered 2D material shows great potential. MXenes is a novel candidate of the 2D family (MXenes described as M n+1 X n T x , where M, X, and T x usually represent the early transition metal, C or N, and adsorbed surface functional groups such as OH, O, and F, where n = 1, 2, or 3). [8] 2D transition metal carbide and nitride MXene (including Ti 3 C 2 T x , Mo 2 CT x , and V 4 C 3 T x ) are excellent electrode materials for supercapacitors due to the high metallic conductivity, excellent cycling stability, and surface chemical groups galore. [9] The preparation of MXene freestanding film by vacuum-assisted filtration is the optimal choice to achieve these properties. [10] For instance, rolled Ti 3 C 2 T x films show a high conductivity of 150 000 S m −1 and gravimetric capacitance Flexible electrodes with excellent energy storage and conversion properties that can be produced by a simple process are highly desirable for supercapacitors. Herein, Cobalt-Nickel double hydroxide (CoNi-DH) micro-nanosheet arrays are prepared uniformly on naturally sedimented Ti 3 C 2 T x films by an etching-deposition-growth process to form a CoNi-DH@Ti 3 C 2 T x heterostructure. The naturally sedimented Ti 3 C 2 T x film serves as the substrate to minimize aggregation of the CoNi-DH nano arrays to enhance the electrical conductivity. Furthermore, the hierarchical structure comprised of the CoNi-DH interconnected nanoarrays promotes electrolyte access. By taking advantage of the excellent electrical conduction and high theoretical specific capacitance, the flexible CoNi-DH@Ti 3 C 2 T x electrode in the supercapacitor delivers a superior specific capacitance of 919.5 F g −1 at 1 A g −1 , and remarkable capacitance retention of 89.6% after 5000 cycles at 20 A g −1 . Density-functional theory calculations are performed to investigate the charge density difference and partial density of states of CoNi-DH@Ti 3 C 2 T x and the theoretical assessment suggests that the chemical bonds between Ti 3 C 2 T x and CoNi-DH are critical to the charge transport, electrical conductivity, and structural stability.