Carrier mobility and density are intrinsically important in nanophoto/electronic devices. Highdielectric-constant coupled polarization-field gate ferroelectrics are frequently studied and partially capable in achieving large-scale tuning of photoresponse, but their light absorption and carrier density seem generally ineffective. This raises questions about whether a similarly high-dielectric-constant paraelectric gate dielectric could enable tuning and how the principles involved could be established. In this study, by deliberately introducing lattice defects in high-dielectric-constant paraelectric, cubic BaTiO 3 (c-BTO) was explored to fabricate MoS 2 photodetectors with ultrahigh detection ability and outstanding field-effect traits. An organic-metal-based spincoating cum annealing method was used for the c-BTO synthesis, with an optimized thickness (300 nm), by introducing lattice defects properly but maintaining a large dielectric constant (55 at 1k Hz) and low dielectric loss (0.06 at 1k Hz), which renders the enhanced visible-light region absorption. As a result of the synergistically enhanced mobility and photoabsorption, the MoS 2 /BTO FET exhibits promising merits, for example, on/off ratio, subthreshold swing, and mobilities for high-performance photodetectors with excellent responsivity (600 AW −1 ) and detectivity (1.25 × 10 12 Jones). Thus, this work facilitates the establishment of a lattice defect induced sub-bandgap absorption landmap for synergistically enhanced photoresponse for high-performance photodetector exploration.