The temperature dependence of deuterium NMR spin-lattice and spin-spin relaxation time data for ethane and ethene adsorbed in zeolite NaA is presented for sorbate loadings in the range 1-4 molecules/cavity. Analytical expressions relating these data to the dynamics of the sorbate molecules are derived. Simultaneous fitting of the temperature dependence of both T-1 and T-2 data for each sorbate loading provides estimates of the correlation time characterizing translational, rotational, and librational motions of the sorbate within the zeolite. The NMR data presented are consistent with ethane having a higher mobility than ethene within the zeolite. Data derived from the NMR study are then used as input to a Monte Carlo lattice dynamics (MCLD) model, which predicts adsorption and transport characteristics of the sorbate-zeolite system. Desorption events from adsorption sites are characterized by a correlation time of the form tau = tau(o) exp[E/(RT)], and the probability of the sorbate attempting an intercage jump process is assumed to be of the form p(w) P-wo exp[-Delta(RT)], where tau(o) and p(wo) are constants and E and Delta are the activation energies characteristic of the respective processes. From the NMR analysis, it is found that ethane transport is characterized by values of tau(o), E, p(wo), and Delta of 2.6 x 10(-9) s, 16 kJ/mol, 0.48, and 7.8 kJ/mol, respectively, while the corresponding values for ethene are 2.0 x 10(-11) s, 27 kJ/mol, 0.105, and 8.5 kJ/mol. The extent of sorbate-sorbate interaction is also quantified and included in the simulation. Predictions of the temperature dependence of ethene adsorption and the concentration dependence of ethene self-diffusivity are shown to be in excellent agreement with existing experimental data. The MCLD model is also used to predict the self-diffusion coefficients of ethane and ethene species within a binary ethane-ethene mixture.