▎ 摘　　要

Facile regulation of magnetic-dielectric synergy is of great importance for the fabrication of microwave ab-sorption (MA) materials. Herein, we propose a polymeric ligand-mediated interface self-assembly strategy to design a series of MA composites using magnetic nanoclusters and graphene nanosheets as building blocks. The employed aromatic polymeric ligand not only allows the assembly of individual nanocrystals into magnetic nanoclusters but also enables their attachment to graphene substrate, resulting in rapid integration of magnetic and dielectric modules at ambient temperature. The straightforward self-assembly enables consecutive MA performances across a wide range of minimum reflection loss that can be greatly increased by 4.3 times. Moreover, the self-assembled nanocomposites exhibit ultrathin MA characteristics with strong reflection loss at an ultrathin thickness of only 1.5 mm and effective frequency bandwidth at an ultrathin thickness of only 1.4 mm. This work provides insights into simple modulation of structure and properties toward ultrathin MA materials.