Recently, van der Waals heterostructure has attracted interest both theoretically and experimentally for their potential applications in photoelectronic devices, photovoltaic devices, plasmonic devices and photocatalysis. Inspired by this, we design a lepidocrocite-type TiO2/GaSe heterostructure. Via first-principles simulations, we show that such a heterostructure is a direct bandgap semiconductor with a strong and broad optical absorption, ranging from visible light to UV region, exhibiting its potential application in photoelectronic and photovoltaic devices. With the planaraveraged electron density difference and Bader charge analysis, the heterostructure shows a strong capacity of enhancing the charge redistribution especially at the interface, prolonging the lifetime of excitons, and hence improving photocatalytic performance. By applying biaxial strain and interlayer coupling, the heterostructure exhibits a direct-indirect bandgap transition and shows a potential for mechanical sensors due to the smooth and linear variation of bandgaps. Furthermore, our result indicates that a lower interlayer distance leads to a stronger charge redistribution. The calculation of irradiating ultrafast on the heterostructure further reveals a semiconductor-metal transition for the heterostructure. Moreover, we find an enhanced induced plasmonic current in the heterostructure under both x-polarized and z-polarized laser, which is beneficial to plasmonic devices designs. Our research provides valuable insight in applying the lepidocrocite-type TiO2/GaSe heterostructure in photoelectronic, photovoltaic, photocatalytic, mechanical sensing and plasmonic realms.