Bifunctional electrocatalysts for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline electrolyte may improve the efficiency of overall water splitting.Nickel cobaltite (NiCo 2 O 4 )has been considered ap romising electrode material for the OER. However, NiCo 2 O 4 that can be used as an electrocatalyst in HER has not been studied yet. Herein, we report self-assembled hierarchical NiCo 2 O 4 hollowm icrocuboids for overall water splitting including both the HER and OER reactions.T he NiCo 2 O 4 electrode shows excellent activity towardo verall water splitting,with 10 mA cm À2 water-splitting current reached by applying just 1.65 Vand 20 mA cm À2 by applying just 1.74 V across the two electrodes.T he synthesis of NiCo 2 O 4 microflowers confirms the importance of structural features for highperformance overall water splitting.Asfossil fuels decline and environmental pollutions aggravate,f uture societies will have to rely on sustainable and regenerative energy sources for development. Water splitting has been widely regarded as ap romising and sustainable approach of producing clean hydrogen fuel from aqueous solutions. [1] However,t he practical applications of water splitting are very limited because splitting reactions,including the anodic oxygen evolution reaction (OER) and the cathodic hydrogen evolution reaction (HER), are strongly uphill with large overpotentials. [2] In alkaline solution, noble-metal oxides (e.g.I ro xides) [3] usually serve as the OER catalysts and NiMo alloy are traditional electrocatalysts for HER. [4] However,t heir large-scale applications are restricted by the high cost of precious metals. [5] It is highly desired to design effective catalysts for water splitting by using non-noble metals.Inthis regard, transition-metal oxides,chalcogenides, and phosphides have been demonstrated as promising electrocatalysts for the OER and HER reactions in water splitting. [1b, 6]