A buckminsterfullerene (C60)-based primary ion beam system has been developed for routine application in TOF-SIMS analysis of organic materials. The ion beam system is described, and its performance is characterized. Nanoamp beam currents of C60+ are obtainable in continuous current mode. C60(2+) can be obtained in pulsed mode. At 10 keV, the beam can be focused to less than 3 microm with 0.1 nA currents. TOF-SIMS studies of a series of molecular solids and a number of polymer systems in monolayer and thick film forms are reported. Very significant enhancement of secondary ion yields, particularly at higher mass, were observed using 10-keV C60+ for all samples other than PTFE, as compared to those observed from 10 keV Ga+ primary ions. Three materials (PS2000, Irganox 1010, PET) were studied in detail to investigate primary ion-induced disappearance (damage) cross sections to determine the increase in secondary ion formation efficiency. The C60 disappearance cross sections observed from monolayer film PS2000 and self-supporting PET film are close to those observed from Ga+. The resulting C60 efficiencies are 30-100 times those observed from gallium. The cross sections observed from C60 bombardment of multilayer molecular solids are approximately 100 times less, such that essentially zero damage sputtering is possible. The resulting efficiencies are > 10(3) greater than from gallium. It is also shown that C60 primary ions do not generate any more low-mass fragments than any other ion beam system does. C60 is shown to be a very favorable ion beam system for TOF-SIMS, delivering high yield, close to 10% total yield, favoring high-mass ions, and on thick samples, offering the possibility of analysis well beyond the static limit.