Designing a functional, conductive metal-organic framework (cMOF) is highly desired. Substantial efforts have been dedicated to increasing the intralayer conjugation of the cMOFs, while less dedication has been made to tuning the interlayer charge transport of the metal-organic nanosheets for the controllable dielectric property. Here, we construct a series of conductive bimetallic organic frameworks of (Zn _x Cu _3-x ) (hexahydroxytriphenylene) ₂ (ZnCu-HHTP) to allow for fine-tuned interlayer spacing of two-dimensional frameworks, by adjusting the ratios of Zn and Cu metal ions. This approach for atomistic interlayer design allows for the finely control of the charge transport, band structure, and dielectric properties of the cMOF. As a result, Zn3Cu1-HHTP, with an optimal dielectric property, exhibits high-efficiency absorption in the gigahertz microwave range, achieving an ultra-strong reflection loss of −81.62 decibels. This study not only advances the understanding of the microstructure-function relationships in cMOFs but also offers a generic nanotechnology–based approach to achieving controllable interlayer spacing in MOFs for the targeted applications.

There is an urgent demand for flexible, lightweight, mechanically robust, excellent electromagnetic interference (EMI) shielding materials. Two-dimensional (2D) transition metal carbides/nitrides (MXenes) have been potential candidates for the construction of excellent EMI shielding materials due to their great electrical electroconductibility, favorable mechanical nature such as flexibility, large aspect ratios, and simple processability in aqueous media. The applicability of MXenes for EMI shielding has been intensively explored; thus, reviewing the relevant research is beneficial for advancing the design of high-performance MXene-based EMI shields. Herein, recent progress in MXene-based macrostructure development is reviewed, including the associated EMI shielding mechanisms. In particular, various structural design strategies for MXene-based EMI shielding materials are highlighted and explored. In the end, the difficulties and views for the future growth of MXene-based EMI shields are proposed. This review aims to drive the growth of high-performance MXene-based EMI shielding macrostructures on basis of rational structural design and the future high-efficiency utilization of MXene.