including catalysis, [2,3] sensing, [4,5] storage and separation, [6,7] devices, [8] drug delivery and imaging. [9] As one of the most valuable forms for practical use, MOF-based films have attracted more and more interest because they could serve as highly versatile, low-energy alternative materials for chemical sensors, separators, and catalysts. [10][11][12] In MOF film-based applications, the selection of MOFs with pores of appropriate size, shape, and chemistry could allow for adsorption and separation with high selectivity. However, the thick MOF films still suffer from low flux due to the low diffusion rates of molecules in the long and narrow channels of MOFs (Figure 1a,b). [13,14] Pioneering efforts have demonstrated that preparing ultrathin MOF nanosheet (NS)-based film is an effective strategy for maximizing the permeance of MOF films. [12] For example, ultrathin Zn 2 (bim) 4 NS-and MAMS-1 NSbased nm-thick molecular sieving membranes showed high gas permeation flux. [15,16] According to Fick's Law, the Knudsen diffusion flow passing through the micropores of MOFs follows the rule: [17] J ∝ 1/L, where J-permeability; L-film thickness. Therefore, the thinner the prepared film, the higher its permeability (Figure 1c). The construction of MOF NSs in very thin layers benefits the permeance of molecules, but restricts mechanical stability and cyclic utilization due to the very low elastic modulus of the MOF NSs. The soft nanosheets are always suffering from severe structure deterioration or fragmentation during exfoliation, application, and recollection. This greatly limits their applications in some cases (Figure 1d). [18,19] Our previous study revealed that while the NSs are assembled into an intersecting structure, the stress or strain can be effectively distributed, thus the NSs-based structure obtaining high mechanical stability. [20] This stimulates us to synthesize thin MOF NSs-based films with high permeance and assemble the MOF NSs into frame film structure with high mechanical stability.Numerous strategies for the fabrication of continuously MOFs films, composed of an uninterrupted, pure layer have been developed. [21] One of the most economical and practical strategies for the large-scale fabrication of MOFs film is the direct conversion of the ceramic precursors films into MOFs films at room temperature. [22][23][24][25] Herein, we design and construct a CuBDC nanosheet-assembled frame (NAF) film using a heteroepitaxial growth method and set it as catalyst. The effective thickness for passage of molecules through the NAF film is reduced to the nanometer level (Figure 1e). Impressively, The engineering of metal-organic frameworks (MOFs) into membranes and films is being investigated, to transform laboratory-synthesized MOFs into industrially viable products for a range of attractive applications. However, rational design and construction of highly permeable MOF thin films, without trade-offs in terms of structural mechanical stability, remains a significant challenge. Herein, a simple, general str...