The development of ultrathin two-dimensional metal-organic framework nanosheets (2D MONs) has recently attracted increasing interest due to their extensive application potential originating from their ultrathin thickness, large surface area, and innumerable accessible surface-active sites. In this frontier article, we highlight the recent developments of 2D MONs for highly efficient heterogeneous catalysts; they can be grouped into three sections in terms of their functions: (i) as catalysts capable of showing outstanding intrinsic reactivity, (ii) as support materials for prevalent catalysts, and (iii) as catalysts with multifunctional catalytic activity for diverse organic transformations. In addition, the present challenges and future opportunities in this field are also discussed.