This study proposes an interface-induced dual-pinning mechanism to enhance low-frequency electromagnetic wave absorption. The researchers constructed a bilayer core-shell structure of NiFe₂O₄ (NFO)@BiFeO₃ (BFO)@polypyrrole (PPy) to create a magnetoelectric bias interface. This interface induces distinct magnetic pinning of the magnetic moment in the ferromagnetic NFO and dielectric pinning of the dipole rotation in PPy. The dual-pinning effect optimizes impedance matching and enhances low-frequency attenuation, leading to improved electromagnetic wave absorption performance. The minimum reflection loss (RL_min) at a thickness of 4.43 mm reaches -65.30 dB (optimal absorption efficiency of 99.99997%), and the effective absorption bandwidth (EAB) almost covers the C-band (4.72–7.04 GHz) with a low filling of 15.0 wt.%. The study demonstrates a mechanism to optimize low-frequency impedance matching with electromagnetic wave loss and provides a pathway for the development of high-performance low-frequency absorbers. The results show that the interface-induced dual-pinning mechanism significantly enhances the absorption efficiency and bandwidth of low-frequency electromagnetic waves. The study also highlights the importance of interface engineering in improving the performance of electromagnetic wave absorbing materials. The findings contribute to the development of advanced materials for electromagnetic wave absorption applications.This study proposes an interface-induced dual-pinning mechanism to enhance low-frequency electromagnetic wave absorption. The researchers constructed a bilayer core-shell structure of NiFe₂O₄ (NFO)@BiFeO₃ (BFO)@polypyrrole (PPy) to create a magnetoelectric bias interface. This interface induces distinct magnetic pinning of the magnetic moment in the ferromagnetic NFO and dielectric pinning of the dipole rotation in PPy. The dual-pinning effect optimizes impedance matching and enhances low-frequency attenuation, leading to improved electromagnetic wave absorption performance. The minimum reflection loss (RL_min) at a thickness of 4.43 mm reaches -65.30 dB (optimal absorption efficiency of 99.99997%), and the effective absorption bandwidth (EAB) almost covers the C-band (4.72–7.04 GHz) with a low filling of 15.0 wt.%. The study demonstrates a mechanism to optimize low-frequency impedance matching with electromagnetic wave loss and provides a pathway for the development of high-performance low-frequency absorbers. The results show that the interface-induced dual-pinning mechanism significantly enhances the absorption efficiency and bandwidth of low-frequency electromagnetic waves. The study also highlights the importance of interface engineering in improving the performance of electromagnetic wave absorbing materials. The findings contribute to the development of advanced materials for electromagnetic wave absorption applications.