Group-10 layered transitional metal dichalcogenides including PtS2, PtSe2 and PtTe2 are excellent potential candidates for optoelectronic devices due to their unique properties such as high carrier mobility, tunable bandgap, stability and flexibility. Large-area platinum diselenide (PtSe2) with semiconducting characteristics is far scarcely investigated. Here, we report on the development of a high performance photodetector based on vertically aligned PtSe2-GaAs heterojunction which exhibited a broadband sensitivity from deep ultraviolet (DUV) to near infrared (NIR) light, with peak sensitivity from 650 to 810 nm. The Ilight/Idark ratio and responsivity of photodetector were 3×10 4 and 262 mA W −1 measured at 808 nm under zero bias voltage. The response speed of τr/τf were 5.5/6.5 μs, which represented the best result achieved for Group-10 TMDs based optoelectronic device thus far. According to first-principle density functional theory, the broad photoresponse ranging from visible to near infrared region is associated with the semiconducting characteristics of PtSe2 which has interstitial Se atoms within the PtSe2 layers. It was also revealed that the PtSe2/GaAs photodetector did not exhibit performance degradation after 6 weeks in air. The generality of the above good results suggests that the vertically aligned PtSe2 is an ideal material for high-performance optoelectronic systems in the future.