We investigated the crystal and electronic structures of ferroelectric Bi 4 Ti 3 O 12 (BiT) single crystalline thin films site-specifically substituted with LaCoO 3 (LCO). The epitaxial films were grown by pulsed laser epitaxy on NdGaO 3 and SrTiO 3 substrates to vary the degree of strain. With increasing the LCO substitution, we observed a systematic increase in the c-axis lattice constant of the Aurivillius phase related with the modification of pseudo-orthorhombic unit cells. These compositional and structural changes resulted in a systematic decrease in the band gap, i.e., the optical transition energy between the oxygen 2p and transition metal 3d states, based on a spectroscopic ellipsometry study. In particular, the Co 3d state seems to largely overlap with the Ti t 2g state, decreasing the band gap.Interestingly, the applied tensile strain facilitates the band gap narrowing, demonstrating that epitaxial strain is a useful tool to tune the electronic structure of ferroelectric transition metal oxides.