Lead halide perovskite (CsPbBr3) quantum dots (QDs) and two-dimensional (2D) layered transition metal dichalcogenides have a significant application in solution-processed optoelectronic devices. Here, we report the oleylamine-assisted exfoliation of TiSe2 nanosheets (NSs) in dichlorobenzene with high concentration and stable dispersion. The functionalized TiSe2 NSs were used to synthesize the solution-processed perovskite CsPbBr3 QD/TiSe2 NS-based nanocomposite. The perovskite QDs and TiSe2 NSs were characterized by different techniques. The strong photoluminescence (PL) quenching and decreased lifetime decay of the nanocomposite indicates efficient charge transfer from photo-excited CsPbBr3 to TiSe2 NSs. The calculated charge-transfer rate constant (KET) from photo-excited CsPbBr3 to TiSe2 NSs increased from 1.50 × 108 to 2.79 × 108 s-1 in different concentrations of TiSe2 NSs (5 to 20 μg mL-1), respectively. Furthermore, the photo-currents of CsPbBr3 QD/TiSe2 NS nanocomposite devices were dramatically enhanced ∼2 times compared to pristine CsPbBr3 QD based devices, which supports the charge transfer and charge separation in nanocomposite devices.