Direct methylation of [60]fullerene via a gas-phase reaction in a CH4/H-2 atmosphere was performed using a modified hot filament chemical vapor deposition method. Pressures were varied from 10 to 60 mbar and the substrate was maintained at 690 degrees C. High-resolution matrix-assisted laser desorption ionization (MALDI) mass spectrometry analysis showed signals corresponding to C60H18-2n(H,CH3)(n). Collision-induced dissociation experiments confirmed a maximum of 18 ligands possible to the [60]fullerene cage.