Composites of ferromagnetic particles and conductive polymers have potential applications in the wave-absorbing stealth technology. In this paper, FeSiAl@polyaniline (FeSiAl@ PANI) composites were prepared through in situ oxidative polymerization. Electromagnetic parameters of the FeSiAl composites were modulated by varying the aniline content. The inhomogeneous interface between amorphous PANI and FeSiAl provides interfacial polarization, charge accumulation, and defects in the PANI layer, which causes dipole polarization and conductive loss, so that multiple loss mechanisms result in the FeSiAl@PANI composites with superior absorbing properties. When 1 g of aniline monomer is added, the lowest reflection loss (RL) can be obtained for the S 1 sample at a thickness of only 1 mm with an RL min value of −37.87 dB. Radar cross-sectional (RCS) simulations using computer simulation technology (CST) for the S 1 sample showed an RCS reduction value of 31.64 dBm 2 . Therefore, the FeSiAl@PANI composite is anticipated to be a candidate material for radar stealth technology and electromagnetic absorption.