take place on the surface or near-surface region of pseudocapacitive materials is particularly paramount to the development of supercapacitors with both high energy density, high rate capability, and long cycle life.Ni(OH) 2 /NiO(OH) couple is the main redox system used in the positive electrodes of alkaline rechargeable batteries, because of its good reversibility and cyclic behavior. [ 5,6 ] Ni(OH) 2 has also attracted great interest as pseudocapacitive materials for supercapacitors due to its high theoretical specifi c pseudocapacitance of 2082 F g −1 (in a potential window of 0.5 V), environmental friendliness, and low cost. [ 7 ] In particular, Ni(OH) 2 in amorphous phase is expected to have better electrochemical effi ciency due to more grain boundaries and ion diffusion channels in the disordered structure compared to the crystalline phase. [ 7,8 ] The key issues of applying Ni(OH) 2 in practical supercapacitors lie in its low electrical conductivity and short cycle life. The electrical conductivity of Ni(OH) 2 is very low at around 10 −15 Ω −1 m −1 . [ 9 ] Thus, the redox reactions can only take place on its surface, and most of Ni(OH) 2 is inaccessible to electrolyte ions and remains as dead volume in supercapacitors. [ 10,11 ] Several approaches have been explored to address the issues caused by the low electrical conductivity of Ni(OH) 2 , including synthesis of porous structures, nanoparticles, thin fi lms, and nanosheets to expose more Ni(OH) 2 surfaces to electrolyte ions, [ 12,13 ] forming Ni(OH) 2 and carbon materials or conducting polymers hybrids to have imbedded conductive networks, [14][15][16][17][18] introducing other metal ions into Ni(OH) 2 to enhance its conductivity. [ 17,19,20 ] Even though these nanoscale engineering approaches can improve the electrical conductivity of Ni(OH) 2 , the constructed nanoscale structures often degrade and Ni ions dissolve into electrolytes after repeated charge/discharge cycles, which can result in short cycle life of supercapacitors. [ 5,13,14,[20][21][22] In this study, with the aim of constructing supercapacitors with both high energy density, good rate capability, and long cycle life, we have designed and synthesized a novel ternary hybrid electrode material comprising of multiwalled carbon nanotubes (MWCNTs), amorphous(amor)-Ni(OH) 2 and poly (3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) as high performance pseudocapacitive materials. Other than the commonly used crystalline Ni(OH) 2 , a thin layer of disordered amor-Ni(OH) 2 was deposited on conductive acidtreated MWCNTs by using a "coordinating etching and precipitating" method, which enabled effi cient redox reactions to take place mostly on the surface of Ni(OH) 2 . To prevent the dissolution of Ni ions into electrolytes and preserve the nanoscale structures amor-Ni(OH) 2 upon long charge/discharge cycles, a conductive polymer layer was further wrapped around the MWCNT/amor-Ni(OH) 2 . Such a unique hybrid architecture design results in Ni(OH) 2 pseudocapacitive materials with ult...