The synthesis of a novel titanocene complex 2a containing a cyclopentadienyl and an indenyl ligand is reported. The complex was prepared in a one-pot procedure from indene and pentamethylene fulvene. The preparation and X-ray structure determination of the tetrahydroindenyl analog 2b is also reported. Catalytic hydrogenation of 2-phenylpyrroline was conducted with the two complexes. It was found that complex 2b catalyzed the reaction at a rate of five times that observed for complex 2a. This rate difference is attributed to the difference in electron density at the metal center.