The parent NaX and KL samples were prepared by hydrothermal crystallization and their corresponding K- and Na-exchanged forms were obtained by post-synthesis modification by conventional ion-exchange technique. NaX, NaKX, KL and NaKL samples were characterized by powder XRD, IR, low temperature nitrogen adsorption and chemical analyses. Their sorption uptake behaviour has been investigated by gravimetric method. The kinetics of sorption using different sorbate probe molecules such as water, benzene and n-hexane was measured at 298 K, at P/P0 = 0.5 for 90 minutes. All the results obtained were discussed in terms of the compositional and structural variations of the adsorbents. Lack of high dimensionality of the pore system, less openness in structure, low average framework oxygen charge and less number of accessible nonframework cations are some of the prominent factors which has resulted in reduced hydro- and organo-philicity in LTL type zeolites as compared to X-type. The size and concentration of the accessible nonframework cations were also found to influence the sorptive properties of these aluminous large pore zeolites. Among all the probe molecules, n-hexane was found to be as a promising probe for differentiating the structural peculiarities especially dimensionality of the pore system.