The interface of transition-metal dichalcogenides (TMDCs) and high-k dielectric transition-metal oxides (TMOs) had triggered umpteen discourses because of the indubitable impact of TMOs in reducing the contact resistances and restraining the Fermi-level pinning for the metal−TMDC contacts. In the present work, we focus on the unresolved tumults of largearea TMDC/TMO interfaces, grown by adopting different techniques. Here, on a pulsed laser-deposited MoS 2 thin film, a layer of TiO 2 is grown by atomic layer deposition (ALD) and pulsed laser deposition (PLD). These two different techniques emanate the layer of TiO 2 with different crystallinities, thicknesses, and interfacial morphologies, subsequently influencing the electronic and optical properties of the interfaces. Contrasting the earlier reports of n-type doping at the exfoliated MoS 2 /TiO 2 interfaces, the large-area MoS 2 /anatase−TiO 2 films had realized a p-type doping of the underneath MoS 2 , manifesting a boost in the extent of p-type doping with increasing thickness of TiO 2 , as emerged from the X-ray photoelectron spectra. Density functional analysis of the MoS 2 /anatase−TiO 2 interfaces, with pristine and interfacial defect configurations, could correlate the interdependence of doping and the terminating atomic surface of TiO 2 on MoS 2 . The optical properties of the interface, encompassing photoluminescence, transient absorption and z-scan two-photon absorption, indicate the presence of defect-induced localized midgap levels in MoS 2 /TiO 2 (PLD) and a relatively defect-free interface in MoS 2 / TiO 2 (ALD), corroborating nicely with the corresponding theoretical analysis. From the investigation of optical properties, we indicate that the MoS 2 /TiO 2 (PLD) interface may act as a promising saturable absorber, having a significant nonlinear response for the sub-band-gap excitations. Moreover, the MoS 2 /TiO 2 (PLD) interface had exemplified better phototransport properties. A potential application of MoS 2 /TiO 2 (PLD) is demonstrated by the fabrication of a p-type phototransistor with the ionic-gel top gate. This endeavor to analyze and perceive the MoS 2 /TiO 2 interface establishes the prospectives of large-area interfaces in the field of optics and optoelectronics.