TS-1 catalysts have been used in olefins epoxidation reactions; however, improving the epoxide selectivity of traditional TS-1 catalysts is a challenge. Here we will discuss how we have been able to achieve this objective by synthesizing TS-1 morphologies with much lower titanium loadings and shorter contact times to limit side reactions. We will first describe the preparation of TS-1@silicalite-1 (egg-shell) catalysts using a secondary growth protocol that places a thin layer of TS-1 on the surface of a silicalite-1 seed crystal. Catalyst testing using n-hexene epoxidation reveals that the egg-shell, which is a pseudo nanosheet of TS-1, exhibits higher selectivity over bulk TS-1. A similar outcome was observed for finned TS-1 prepared by secondary growth wherein nanosized TS-1 protrusions (fins, ca. 50 nm) epitaxially grow on the surfaces of silicalite-1 seed crystals. This technique has been demonstrated for a series of aluminosilicate zeolites (MFI, MEL, FER) where fins enhance internal diffusion, thereby extending catalyst lifetime. For n-hexene epoxidation, fins give reactant molecules rapid access to Ti sites while minimizing contact time, leading to enhanced catalyst selectivity that is comparable to the egg shell configuration.