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In this study, a facile and inexpensive and self-assembled strategy to massively fabricate Ni/Co layered double hydroxides (LDHs) is developed under mild reaction conditions (55 °C). The resulting composite material displays a special three-dimensional hierarchical microsphere structure with well-defined flower-like configuration. The fabrication mechanism can be ascribed to stepwise and regular reaction process of nanoparticles and nanosheets gradually growing to nanopetals and then assembling into flower-like microspheres, based on the systematically investigation of various reaction factors including the Ni:Co feeding ratio, the reaction time and the initial pH-value. Because of its large surface, ultrathin feature and synergetic results of this Ni/Co LDHs nanosheets (20 nm), these Ni/Co-LDHs microspheres deliver an excellent capacitance value about 2228 F·g^–1 (1 A·g^–1). An all-solid-state flexible …