Visible Raman spectroscopy excited at 532 nm was used to characterize the carbon bonding in tetrahedral amorphous carbon (ta-C) films. The vibrational modes of the sp3 bonding in ta-C films were revealed directly. An additional Raman band occurring below 1350 cm−1 was observed. It consisted of two features centered on ∼1270 and ∼1170 cm−1, which were associated with sp3 bond stretching. The observed sp3 related Raman spectrum approached the vibrational density of states of amorphous diamond.