This communication reports the first integration of two significant concepts, macromolecular helicity-derived chirality, and magneticity in one single microsphere entity. The novel chiral magnetic composite microspheres consisted of magnetic Fe3O4 nanoparticles and optically active helical substituted polyacetylene. Therefore, they exhibited both remarkable optical activity and magneticity. The microspheres adsorbed (R)-(+)-1-phenylethylamine much more quickly than the other enantiomer, demonstrating the potential applications of the chiral magnetic composite microspheres in chiral recognition and chiral resolution.