FeCoNi-coated PMMA (FeCoNi@PMMA) core-shell structures prepared by an electroless plating process were investigated in this study. Further, we fabricated FeCoNi@PMMA in polydimethylsiloxane sheets with volume fractions of fillers from 10 vol% to 25 vol% to evaluate electromagnetic wave absorption performance. Subsequently, results were compared with those of carbonyl iron particles (CIP). The maximum reflection loss (RL) of FeCoNi@PMMA composite (25 vol%) reached a value of -37.2 dB at 12.2 GHz with a thickness of 1.5 mm and a broad absorption bandwidth (RL <= -10 dB) of 4.5 GHz, attributed to strong dielectric and magnetic losses. Though the microwave absorption performance of the core-shell structured FeCoNi@PMMA composites is similar to that of CIP composites, the weight fraction of FeCoNi@PMMA is reduced about 38% compared with CIP with the same volume fraction (25 vol%). These results indicate that FeCoNi@PMMA is a lightweight material and a good candidate for high-performance microwave-absorbing devices.