2D Metal Organic Framework Nanosheet: A Universal Platform Promoting Highly Efficient Visible‐Light‐Induced Hydrogen Production

2D metal organic frameworks (MOF) have received tremendous attention due to their organic–inorganic hybrid nature, large surface area, highly exposed active sites, and ultrathin thickness. However, the application of 2D MOF in light‐to‐hydrogen (H2) conversion is rarely reported. Here, a novel 2D MOF [Ni(phen)(oba)]n·0.5nH2O (phen = 1,10‐phenanthroline, oba = 4,4′‐oxybis(benzoate)) is for the first time employed as a general, high‐performance, and earth‐abundant platform to support CdS or Zn0.8Cd0.2S for achieving tremendously improved visible‐light‐induced H2‐production activity. Particularly, the CdS‐loaded 2D MOF exhibits an excellent H2‐production activity of 45 201 µmol h−1 g−1, even exceeding that of Pt‐loaded CdS by 185%. Advanced characterizations, e.g., synchrotron‐based X‐ray absorption near edge structure, and theoretical calculations disclose that the interactive nature between 2D MOF and CdS, combined with the high surface area, abundant reactive centers, and favorable band structure of 2D MOFs, synergistically contribute to this distinguished photocatalytic performance. The work not only demonstrates that the earth‐abundant 2D MOF can serve as a versatile and effective platform supporting metal sulfides to boost their photocatalytic H2‐production performance without noble‐metal co‐catalysts, but also paves avenues to the design and synthesis of 2D‐MOF‐based heterostructures for catalysis and electronics applications. Earth‐abundant, two‐dimensional (2D) Ni‐based metal organic framework (MOF) nanosheets serve as a versatile and highly active platform supporting metal sulfides for highly efficient, visible‐light‐photocatalytic H2 production. The advanced characterizations and theoretical calculations confirm that the interfacial electronic coupling, large surface area, numerous reactive centers, and favorable band structure of 2D MOF together contribute to the outstanding photocatalytic activity.