The study explores the design of conductive metal-organic frameworks (cMOFs) with fine-tuned interlayer spacing to enhance microwave absorption properties. The researchers synthesized a series of bimetallic cMOFs, (Zn,Cu2-x) (hexahydroxytriphenylene)2 (ZnCu-HHTP), by adjusting the ratios of Zn and Cu metal ions, which allows for precise control over the interlayer spacing. This approach enables the tuning of charge transport, band structure, and dielectric properties. Among the synthesized cMOFs, Zn3Cu1-HHTP exhibits optimal dielectric properties, achieving high-efficiency microwave absorption in the gigahertz range with an ultra-strong reflection loss of −81.62 decibels. The study not only advances the understanding of microstructure-function relationships in cMOFs but also offers a generic nanotechnology-based method for achieving controllable interlayer spacing in MOFs for targeted applications.The study explores the design of conductive metal-organic frameworks (cMOFs) with fine-tuned interlayer spacing to enhance microwave absorption properties. The researchers synthesized a series of bimetallic cMOFs, (Zn,Cu2-x) (hexahydroxytriphenylene)2 (ZnCu-HHTP), by adjusting the ratios of Zn and Cu metal ions, which allows for precise control over the interlayer spacing. This approach enables the tuning of charge transport, band structure, and dielectric properties. Among the synthesized cMOFs, Zn3Cu1-HHTP exhibits optimal dielectric properties, achieving high-efficiency microwave absorption in the gigahertz range with an ultra-strong reflection loss of −81.62 decibels. The study not only advances the understanding of microstructure-function relationships in cMOFs but also offers a generic nanotechnology-based method for achieving controllable interlayer spacing in MOFs for targeted applications.