Optically active helical substituted (co)polyacetylenes containing pendent pyrene groups are prepared and then noncovalently immobilized on graphene via - interactions. The resulting graphene composite is characterized by XRD, FTIR, Raman, circular dichroism, UV-vis absorption, TEM, TGA, and fluorescent spectroscopy techniques. The helical polyacetylene endows graphene with the desired optical activity. Also interestingly, the dispersibility of the functionalized graphene in tetrahydrofuran is remarkably improved due to the presence of the helical polymer chains. The present methodology opens new opportunities and serves as a versatile platform toward preparing novel graphene-based materials.