Precise assembly of the cytoskeleton (e.g., actin, tubulin, and intermediate filaments) is of great importance for stem cell polarization and tissue regeneration. Recently, artificial manipulation of cytoskeleton assembly for remodeling stem cell polarization and ultimate cell fates attracts more and more interest of both chemists and biologists. Herein, it is reported the magnetic field-directed formation of biocompatible supramolecular polymeric nanofibers composed of two subunits: a β-cyclodextrin-bearing hyaluronic acid host polymer (HACD) and magnetic nanoparticles modified with actin-binding peptide and adamantane (MS-ABPAda). Transmission electron microscopy indicated that when HACD and MS-ABPAda were exposed to a magnetic field, they self-assembled into long nanofibers along the direction of the magnetic field, and the rate of nanofiber formation was linearly correlated with the strength of the magnetic field. Interestingly, when incubated with dental pulp stem cells, the nanofibers specifically drove tip extension and polarization of the cells, a phenomenon that can be attributed to targeting of actin-binding peptide to the actin cytoskeleton and subsequent polarization of the nanofibers. The successful application of these magnetic field-responsive supramolecular polymers on accurately driving polarization of mammalian cells is expected to be of great value for artificially manipulating cell fate and developing intelligent responsive materials in regenerative medicine.