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Using vapor phase transformation to synthesize template‐directed metal–organic frameworks (MOFs) shows great promise as an approach to avoid the shortcomings of solution‐based strategies. However, among current research, either the products are confined to zeolitic imidazolate frameworks or the conversion technologies are limited to complex processes such as chemical vapor deposition. Here, a well‐designed sublimation‐vapor phase pseudomorphic transformation method is reported to fabricate vertically aligned nanosheet arrays of NiFe‐based MOFs with a uniform and controlled thickness, derived from NiFe‐layered double hydroxides. Benefiting from the optimized morphology and the high intrinsic activity originating from the synergistic coupling effect of NiFe metal clusters, the as‐prepared MOF electrocatalyst displays a superior oxygen evolution reaction performance, requiring an overpotential of 318 mV at 50 mA cm−2 with a Tafel slope of only 47 mV dec−1. Furthermore, a string of metal oxide‐MOFs are obtained, demonstrating the universality of this strategy. By observing the different stages of transformation, the transformation and growth mechanism of MOF crystals is unveiled for the first time. These findings may inspire the exploration and preparation of more species of MOFs, further broadening their application areas. [ABSTRACT FROM AUTHOR]