Polypyrrole (PPy)-coated magnetite (Fe 3 O 4 ) hybrid particles were synthesized under sonication. PPy was coated on the surface of Fe 3 O 4 microspheres, whereas pyrrole monomers filled the interior of the Fe 3 O 4 particles and were then polymerized. The structure of the Fe 3 O 4 -PPy microspheres was confirmed by transmission electron microscopy. The electric and magnetic properties were confirmed by optical microscopy and vibrating sample magnetometry, respectively. The suspension of the Fe 3 O 4 -PPy composite microspheres dispersed in silicone oil exhibited both electrorheological and magnetorheological properties when measured using a rotational rheometer under an applied electric and magnetic field, respectively.