3268 wileyonlinelibrary.com inorganic nodes in MOFs can be intrinsic active sites for catalysis, e.g., copperbased MOFs have been demonstrated as an excellent solid Lewis acid catalyst for a few reactions; [ 4,7 ] (ii) extrinsic functional species (e.g., nanoparticles) can be introduced to MOFs structure, either on the external surfaces or inside the bulks or shells of MOFs. Various catalytic nanoparticles have been successfully incorporated into different MOFs matrices, including Au, Ag, Pt, Cu, or their combination etc.; [8][9][10] and (iii) MOFs also serve as solid precursors for metal or metaloxide catalysts due to their high metal density within the frameworks and easy transformation. Many porous transition metal oxides, such as CuO, Cu 2 O, Mn 2 O 3 , Mn 3 O 4 , Co 3 O 4 , and ZnO among others, have been derived through thermolysis under controlled atmospheres. [11][12][13][14][15][16] For example, porous CuO hollow architectures with perfect octahedral shape were prepared by annealing HKUST-1 precursor in fl owing air. [ 12 ] Moreover, zeolitic imidazolate framework-67 (ZIF-67) was used to design and generate Co 3 O 4 or structurally more complex Co 3 O 4 /NiCo 2 O 4 . [ 13,14 ] Although increasing research attention has been paid to the catalytic applications of MOFs, to our knowledge, shapes of the studied MOFs are mostly followed in 3D isotropic polyhedrons (i.e., high symmetric MOF crystals with sizes greater than 100 nm), and the catalytic systems derived from MOFs with anisotropic shapes such as nanofi bers or nanosheets with a dimension(s) less than 10 nm have seldom been explored.Similar to many inorganic nanomaterials, tailoring of size and shape is essential to customize MOFs for specifi c applications according to the principle of "structure dictates function." [ 17 ] Although a fi ne control over the size and size-distribution of MOFs has been realized, e.g., in the range of 100 nm to several micrometers, [ 18 ] fashioning MOFs into desired shapes for specifi c applications remain to be challenging. Nevertheless, several attempts to the architectural control of MOFs shapes have recently appeared in the literature, ranging from 1D, 2D to 3D nanostructures. [ 19,20 ] For example, nanosheets of MOFs as molecular sieving membranes for gas separation have been made in two recent reports, [ 21,22 ] which achieved much higher separation selectivity than MOFs in other