The vibrational predissociation of van der Waals complexes of anthracene-Ar(n) (n = 1,2,3), isolated in a supersonic expansion, has been studied following excitation to single vibrational levels (12(0)1, 10(0)1, 12(0)2, 6(0)1 in S1. Using picosecond time-resolved fluorescence spectroscopy, the intramolecular vibrational-energy redistribution (IVR) and the vibrational predissociation (VP) dynamics are studied and related to the character of the mode and its energy. The IVR and VP rates are also discussed in relation to the cluster size.