With the aid of molecular simulation techniques (molecular dynamics, grand-canonical Monte Carlo, and reactive flux correlation function RFCF), the influence of the external surface on the equilibrium permeation of methane and ethane into and out of an AFI-type zeolite crystal has been studied. In particular, "extended dynamically corrected transition state theory", which has been proven to describe the transport of tracers in periodic crystals correctly, has been applied to surface problems. The results suggest that the molecules follow paths that are close to the pore wall in the interior and also at the crystal surface. Moreover, the recrossing rate at the surface turns out to be non-negligible, yet, in contrast to the intracrystalline recrossing rate, remains almost constant over loading which gives indication to diffusive barrier crossing at the crystal surface. As a consequence of very different adsorption and desorption barriers, the corresponding permeabilities are shown to be not equal for one and the same condition (T and p). The critical crystal length, beyond which surface effects can be certainly neglected, is computed on basis of flux densities. Entrance/exit effects, in the present cases, are practically important solely for ethane at low pressures. The influence of the type of external surface on the surface flux is, hereby, rather small, because the transport at the surface is controlled by the slow supply from the gas phase. This has been evidenced by a simplified thermodynamic model that has been derived within this work and which is based on rapidly assessable simulation data. Finally, we propose a procedure for estimating the importance of different factors that have an impact on surface effects. © 2010 American Chemical Society.