We demonstrate vibronic excitation combined with spectrally resolved zero phonon line detection of single terrylenediimide (TDI) molecules in both the Shpol'skii matrix hexadecane and the polymer PMMA at cryogenic temperatures. Spectral jumps as large as 80 cm(-1) are recorded with a 1 s time resolution. This technique does not require a weak electron-phonon coupling, and promises applications in spectroscopy of a wide-range of single nanostructures in amorphous hosts including fluorescing proteins. Vibronic excitation is also used to determine vibrational spectra of the excited state of single TDI molecules. (C) 2003 American Institute of Physics.