Molecular dynamics (MD) simulations of the glass-forming liquid Ca0.4K0.6(NO3)1.4 (CKN) have been performed at several temperatures from a liquid state at 800 K down to a glassy state at 150 K. The well-known Ewald summation method of handling the long-range electrostatic interactions has been replaced by the recently proposed method of truncated shifted Coulomb potential (Wolf; et al. J. Chem. Phys. 1999, 10, 8254). Some comparisons between dynamical properties of liquid CKN simulated with either of these methods are provided. A previously introduced polarizable fluctuating charge model (FCM) for the nitrate anion (Ribeiro, M. C. C. Phys. Rev. B 2000, 61, 3297) has been used. It is shown that the FCM is an improvement on the nonpolarizable rigid ion model (RIM) counterpart as the glass transition temperature Tg of the system simulated with the FCM is in better agreement with the experimental calorimetric value (Tg ≈ 475, 380, and 335 K for the RIM, FCM, and experiment, respectively). Reorientational time correlation functions, P2(t), are first analyzed as in previous Raman spectroscopy investigations (Jacobsson; et al. J. Non-Cryst. Solids 1994, 172−174, 161), where the reorientational relaxation time, τor, was obtained from the short time decay of P2(t). Excellent agreement between experimental and calculated τor has been found, including the Arrhenius dependence of τor across Tg. It is shown, however, that the above analysis of the experimental P2(t), where only the short time decay is available, is misleading. Contrary to the Raman results, a marked change in activation energy across Tg is obtained when the long time decay of the calculated P2(t) is considered. The temperature dependence of τor is further compared with the diffusion coefficient, D, and the structural α-relaxation time, τα, obtained from the self-part of the intermediate scattering function. The hierarchy of the decoupling between τor, D, and τα as CKN is cooled to Tg is shown.