The Raman spectrum of buckyferrocene (Fe(C 60 (CH 3 ) 5 )C 5 H 5 ) changes during laser irradiation at 532nm. A peak at 1465cm −1 decreases and a new peak at 1452cm −1 emerges, which resembles the change in the ‘pentagonal pinch mode’ during the photopolymerization of C 60 . Photoinduced polymerization is strongly suggested because fragments from the buckyferrocene dimers are observed during the mass spectroscopy of laser desorbed solid samples. The rate constants of the photoinduced change for the powder crystals were determined at various photon intensities, and linearity was observed. The photoinduced change seems to occur extremely fast in densely packed buckyferrocene films fabricated by vacuum deposition.