The dynamics of vibrational energy relaxation of highly excited molecular iodine in three monatomic solvents is studied via stochastic classical trajectory simulations based on the molecular timescale generalized Langevin equation (MTGLE) of motion for liquid state chemical reactions [S. A. Adelman, J. Chem. Phys. 73, 3145 (1980)]. Also presented for comparison purposes are parallel studies based on a matrix Langevin equation of motion characterized by friction coefficients which depend on the instantaneous I2 internuclear separation R. The qualitative features of the energy relaxation may be interpreted as effects arising from modifications of the solute dynamics due to molecular timescale correlations between its motion and that of its solvation shells. Such dynamical solvent effects are realistically described by the MTGLE equation of motion but not by the Langevin equation. Thus, for example, the marked slowdown of the rate of I2 energy relaxtion in simple solvents when the I2 vibrational quantum number drops below a solvent-dependent critical value, earlier predicted by Nesbitt and Hynes, is predicted by MTGLE dynamics but not by Langevin dynamics. Finally, practical algorithms for numerically constructing the MTGLE and Langevin equations for specific solute–solvent systems are presented.