Economizing Production of Diverse 2D Layered Metal Hydroxides for Efficient Overall Water Splitting

2D layered metal hydroxides (LMH) are promising materials for electrochemical energy conversion and storage. Compared with exfoliation of bulk layered materials, wet chemistry synthesis of 2D LMH materials under mild conditions still remains a big challenge. Here, an “MgO‐mediated strategy” for mass production of various 2D LMH nanosheets is presented by hydrolyzing MgO in metal salt aqueous solutions at room temperature. Benefiting from this economical and scalable strategy, ultrathin LMH nanosheets (M = Ni, Fe, Co, NiFe, and NiCo) and their derivatives (e.g., metal oxides and sulfides) can be synthesized in high yields. More importantly, this strategy opens up opportunities to fabricate hierarchically structured LMH nanosheets, resulting in high‐performance electrocatalysts for the oxygen‐ and hydrogen‐evolution reactions to realize stable overall water splitting with a low cell voltage of 1.55 V at 10 mA cm−2. This work provides a powerful platform for the synthesis and applications of 2D materials. A facile, low‐cost, and versatile MgO‐mediated strategy is developed for the mass production of 2D transition‐metal hydroxides nanosheets and their derivatives. Hierarchically structured oxygen‐ and hydrogen‐evolution electrocatalysts designed based on this strategy show excellent activities and stabilities for overall water splitting.