Femtosecond laser studies have been performed to investigate the initial photodissociation reactions of I-2-mesitylene charge transfer complexes. Photodissociation occurs along both the I-2-mesitylene "bond" and the I-I bond with a branching ratio of 2:3 for the two reaction coordinates. Following excitation at 400 nm, geminate recombination occurs along both reaction coordinates. The reformed I-2-mesitylene complexes are formed vibrationally hot and relax on a time scale of 13 ps. The I-mesityfene spectrum is fully developed within 500 fs of the pump pulse. Approximately 40% of the I-mesitylene complexes undergo geminate recombination on a time scale of 14 ps. Most of the remaining complexes recombine with their original partners on a time scale of 400 ps. The initial anisotropy of the photoproduct absorption is 0.09+/-0.02. This low anisotropy is a direct result of the geometry of the complex and nature of the electronic transition rather than indicative of ultrafast motion toward an asymmetric transition state preceding dissociation.