Two novel and isostructural Ni-based MOFs with topological symbol of 4(22).5(4).6(2), namely [Ni-2(TATB)2(L)2(H2O)], have successfully synthesized, where L is the flexibly N-donor bid (1,10-bisimidazoledecane) or btd (1,10-bistriazoledecane) linker and TATB is the deprotonation mode from 4,4',4 ''-s-triazine-2,4,6-triyl-tribenzoic acid (H(3)TATB). Two types of left- and right-handed helical channels with mean diameter of 11 angstrom results in large void space in 3D network. When directly use as electrode materials, the as-synthesized Ni-MOFs single-crystal electrodes behave as pseudo-capacitor and deliver high gravimetric capacitance with superior energy deliverable ability and cycling stability. For example, the maximum gravimetric capacitance is 705 F g(-1) with the energy density of 29.6 Wh kg(-1) at a current density of 1 A g(-1). Even after 5000 continuous cycles, the capacitance retention maintains at 92.1%. The good electrochemical performance should be ascribed to the 1D helical channels facilitating the diffusion of OH-. Furthermore, the low bulk solution (0.46 and 0.50 Omega) and charge-transfer resistances accelerate the contact between OH and active species in the electrode, and consequently result in efficiency Faradaic reaction. This work opens a new way for the directly application of 3D topological MOFs single-crystal with novel interior structures especially porous and channel-like architectures in electronic energy storage field.