Constructing hybrid metal-organic frameworks (MOFs) demonstrates significant potential to improve electromagnetic wave (EMW) absorption performance by leveraging synergistic effects between composition and structure, addressing challenges in tuning electromagnetic parameters of single-composition MOFs. This study proposes a sophisticated strategy involving sulfidation-interface growth-reassembly: sulfide nanoparticles form by sulfidating the core (CoFe-MIL-88A), and then ZIF-67 guests grow and reassemble on the sulfided host MOF, resulting in a layered EMW absorption material. The composite material integrates synergistic effects, which include high conductive loss and defect/interface/dipole polarization induced by N and S atom doping. The CFSNC composite material outperforms previously published values, achieving a minimum reflection loss (RLmin) of −65.96 dB and an effective absorption bandwidth (EAB) of 6.15 GHz with a thickness of merely 2 mm. Simulation calculations of the real far-field radar cross-section (RCS) further validate its practical application potential. This work introduces novel ideas and methods for designing and preparing high-performance EMW absorption materials, offering both theoretical insights and practical applications.