Carbon nanoparticles (CNPs) derived from metal− organic frameworks (ZIF-8) are synthesized, which are further selfassembled into mono-or bilayer superstructures for electromagnetic (EM) wave absorption. Furthermore, the effect of ZIF-8 morphology (cubic or rhombic dodecahedral) on the superstructure and EM absorption performance of CNPs is investigated. The as-prepared cubic bilayer superstructure exhibits a higher BET surface area of 526.1 m 2 /g and a higher pore volume of 0.232 cm 3 /g than the rhombic dodecahedral monolayer superstructure (30.0 m 2 /g and 0.051 cm 3 /g, respectively). As a result, the two-dimensional CNPs with a bilayer structure are able to deliver the highest EM absorption performance with an effective absorption bandwidth of 6.2 GHz at a thickness of merely 2.4 mm. This work provides a new approach to designing and preparing highperformance EM wave absorption materials.