mixed-metal hydroxide compounds such as Ni-Al, [ 3 ] Co-Ni, [4][5][6][7][8][9][10] Mn-Co, [ 11 ] Co-Ru, [ 12 ] Ni-Co-Cu, [ 13 ] and Ni-Co-Zn [ 14 ] have advantages over single-composition compounds as positive electrode materials for supercapacitors because mixed-metal compounds greatly promote the integrated electrochemical performance. [15][16][17][18] Almost all efforts in this fi eld have been directed towards crystalline mixed-metal hydroxide materials because these compounds have superior electrochemical performance with high specifi c capacitance, excellent rate capability, high energy density, and high power density. [4][5][6][7][8][9][10]19,20 ] However, supercapacitors made from crystalline compounds usually exhibit a very poor or short cycle life, [4][5][6][7][8][9][10] which makes their practical use limited. Typically, the cycling stability of a Ni(OH) 2 -Co(OH) 2 -graphene asymmetric supercapacitor shows a 70% retention after 1000 cycles. [ 8 ] Therefore, increasing the cycle life of mixed-metal hydroxide materials is a signifi cant challenge in supercapacitor applications.Although most positive electrode materials are based on crystalline mixed-metal hydroxides high activities can also be achieved with amorphous phases. It has been shown that the integrated electrochemical performance of amorphous metal hydroxides, such as Ni(OH) 2 and Co(OH) 2 , is commensurate with the crystallinity of the materials in the supercapacitor. [ 21,22 ] Considering the excellent electrochemical performance of crystalline mixed-metal hydroxide electrodes several benefi ts should be realizable by the development of amorphous mixed-metal hydroxide electrodes. However, commonly used methods for the production of amorphous oxide materials are not typically amenable to amorphous mixed-metal hydroxides. [ 18 ] We thus present a simple, facile, and chemically clean electrochemical method (experimental details in the Experimental Section and in Supporting Information S1) to prepare amorphous phases of mixed-metal hydroxides. They exhibited excellent performances as positive supercapacitor electrodes and a fabricated device showed a long-term cycling stability characterized by 94% retention after 20 000 cycles. This proof-of-principle investigation using amorphous mixed-metal hydroxides (amorphous Ni-Co-Fe hydroxide) demonstrates the broad applicability Supercapacitors or electrochemical capacitors, as energy storage devices, require very stable positive electrode materials for useful applications. Although most positive electrodes are based on crystalline mixed-metal hydroxides, their pseudocapacitors usually perform poorly or have a short cycle life. High activities can be achieved with amorphous phases. Methods to produce amorphous materials are also not typically amenable towards mixed-metal compositions. It is demonstrated that electrochemistry in an ambient environment can be used to produce a series of amorphous mixedmetal hydroxides with a homogeneous distribution of metals for use as positive electrode materials in a s...