LAUSR

Metal–organic framework (MOF) derivatives promise great potential in energy storage and conversion because of their excellent tunability in both the active metal sites, organic links, and the overall structures down to atomic and up to mesoscale. Nevertheless, a big challenge is to precisely control and thoroughly understand the actual MOF‐to‐derivative conversion process to realize the template‐free synthesis of the MOF‐derived ordered mesoporous materials. Here, a class of ordered mesoporous N‐doped carbon nanoflakes is presented with slit‐shaped pores synthesized by one‐step pyrolysis of Zn1Cux–MOF, where the Cu doping plays a critically important direction‐inducing function on the dissociation of organic ligands during the pyrolysis. Benefiting from the uniquely ordered mesoporous structure and large specific surface area (910 m2 g−1), the Zn1Cux–MOF‐derived ordered mesoporous carbon nanoflakes present outstanding electrochemical storage performance for multivalent metal ions, such as Mg2+, Ca2+, Co2+, Ni2+, Al3+, and Zn2+, demonstrating the universal nature of the slit‐shaped pores in enabling the multivalent metal ions for energy storage. Moreover, the assembled flexible Zn‐ion hybrid supercapacitor (ZHSC) delivers a high specific capacity of 134 mAh g−1 at 0.5 A g−1, excellent cycling and mechanical stability, showing great application potential in the new generation energy storage devices.