Spatiotemporal modulation of microtubules by light has become an important aspect of the biological and nanotechnological applications of microtubules. We previously developed a Tau‐derived peptide as a binding unit to the inside of microtubules. Here, we conjugated the Tau‐derived peptide to spiropyran, which is reversibly converted to merocyanine by light, as a reversible photocontrol system to stabilize microtubules. Among the synthesized peptides with spiropyran/merocyanine at different positions, several peptides were bound to the inside of microtubules and stabilized the structures of microtubules. The peptide with spiropyran at the N‐terminus induced polymerization and stabilization of microtubules, whereas the same peptide with the merocyanine form did not exert these effects. Reversible formation of microtubules/tubulin aggregates was achieved using the peptide with spiropyran conjugated at the N‐terminus and irradiation with UV and visible light. Spiropyran‐conjugated Tau‐derived peptides would be useful for spatiotemporal modulation of microtubule stability through reversible photocontrol of binding.