Structural design and interface regulation are useful strategies for achieving strong electromagnetic wave absorption (EMWA) and broad effective absorption bandwidth (EAB). Herein, a monomer-mediated strategy is employed to control the growth of covalent organic framework (COF) wrapping flower-shaped Gd-doped FeNi3 (GFN), and a novel raspberry-like absorbent based on biomimetic design is fabricated by thermal catalysis. Further, a unique dielectric-magnetic synergistic system is constructed by utilizing the COF-derived nitrogen-doped porous carbon (NPC) as the shell and anisotropic GFN as the core. The electromagnetic parameters of the GFN@NPC composites can be tuned by adjusting the proportions of GFN and NPC. Off-axis electron holography results further clarify the interface polarization and microscale magnetic interactions affecting the EMW loss mechanism. As a result, the GFN@NPC samples exhibit broad EMWA performance. The EAB values of all GFN@NPC composites reach up to 6.0 GHz, with the GFN@NPC-2 sample showing a minimum reflection loss (RLmin) of -69.6 dB at 1.68 mm. In addition, GFN@NPC-2 achieves a maximum radar cross-section (RCS) reduction of 29.75 dB·m2. A multi-layer gradient structure is also constructed using metamaterial simulation to achieve an ultra-wide EAB of 12.24 GHz. Overall, this work provides a novel bio-inspired design strategy to develop high-performance EMWA materials.