The crystal morphology of silicalite-1 was adjusted through a microemulsion-based hydrothermal synthesis. The surfactant cetyltrimethylammonium bromide (CTAB) with cosurfactant butanol was used to form water-in-oil microemulsions containing the silicalite-1 synthesis gel. The crystal morphology of silicalite-1 was adjusted from coffin-shaped to novel rod-shaped and to irregular-shaped nanoparticles by varying the microemulsion composition. Silicalite-1 synthesized in the microemulsion has a smaller size and a more narrow size distribution than that produced by conventional synthesis without the microemulsion. The novel morphology of silicalite-1 may facilitate assembly into films and find applications in separation and catalysis.