The synthesis of the medium-pore zeolite ZSM-57 in the presence of sodium and N, N,N,N', N', N'-hexaethylpentanediammonium cations is described. Under the synthesis conditions studied here, crystallization of pure ZSM-57 was possible only from synthesis mixtures with a very narrow range of SiO2/Al2O3 and NaOH/SiO2 ratios. The catalytic properties of H-ZSM-57 are evaluated for the skeletal isomerization of l-butene to isobutene and the cracking of n-octane and compared to those obtained from H-ZSM-5 and H-ZSM-35 with the same pore architecture but different pore sizes. A high initial 1-butene conversion is observed for H-ZSM-57, while its selectivity to isobutene is much lower than that of H-ZSM-35. This trend remains almost unchanged with time on stream. Thus, the nonselective behavior of H-ZSM-57 for isobutene formation may be due not only to the presence of very strong acid sites in this zeolite as evidenced by ammonia TPD experiments, but also to its channel intersections that are large enough to allow undesired side reactions such as 1-butene dimerization followed by cracking to light olefins. By contrast, H-ZSM-57 shows considerably higher n-octane cracking activity than ZSM-5 known as one of the most active catalysts for this reaction. However, it is found that the poisoning of strong acid sites in H-ZSM-57 by coke formation occurs within the pores, leading to a continuous decrease in n-octane conversion. Such an aging feature of ZSM-57 suggests that medium-pore zeolites with intersecting channels of two different pore sizes may be less stable as acid catalysts than those with uniform pore size, due to the geometrical constraints imposed by the dual pore system, even in the case that their 10-ring pore sizes are similar to each other.