C60 and C70 were synthesized and purified according to published procedures. Both nanosecond and picosecond laser desorption from coated substrates gave copious positive and negative ions. Mass spectra (TOF and FTMS) with excellent signal to noise, showing only the C60 and C70 mass peaks, have been observed. Well-resolved isotopic structure was seen in the FTMS spectra in agreement with the natural abundance of carbon. Laser desorption and multiphoton ionization/photodissociation of the neutral species, as well as electronic absorption, FTIR, and fluorescence spectra, have been obtained.