The post-synthetic incorporation of titanium in the borosilicate SSZ-33 and the direct synthesis of an aluminum-free titanium-containing zeolite Beta (Ti-Beta) are reported. These materials are characterized by X-ray powder diffraction (XRD), Fourier transform infrared (FTIR), FT-Raman, and diffuse reflectance ultraviolet (DR-UV) spectroscopies. The molecular sieves are shown to catalyze the epoxidation of various olefins using aqueous hydrogen peroxide as the oxidant. The physicochemical properties as found by the characterization methods are correlated to the catalytic data and the results compared to a high quality sample of TS-1. The modified SSZ-33 samples contain titanium primarily in the form of isolated tetrahedrally coordinated Ti atoms, although some extra-framework Ti is observed by Raman and DR-UV spectroscopies. Ti-Beta samples show no evidence of extra-framework titanium. For the epoxidation of cis-cyclooctene, the Ti-Beta catalysts give quantitative conversion to epoxide, and both the Ti-Beta and Ti-SSZ-33 catalysts are able to epoxidize substrates too large to be oxidized by TS-1.