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Ultrathin sheets of two-dimensional (2D) materials like transition metal dichalcogenides have attracted strong attention as components of high-performance light-harvesting devices. Here, we report the implementation of Schottky junction-based photovoltaic devices through site-selective surface doping of few-layer WSe2 in lateral contact configuration. Specifically, whereas the drain region is covered by a strong molecular p-type dopant (NDP-9) to achieve an Ohmic contact, the source region is coated with an Al2O3 layer, which causes local n-type doping and correspondingly an increase of the Schottky barrier at the contact. By scanning photocurrent microscopy using green laser light, it could be confirmed that photocurent generation is restricted to the region around the source contact. The local photoinduced charge separation is associated with a photoresponsivity of up to 20 mA W–1 and an external quantum efficiency of up to 1.3%. The demonstrated device concept should be easily transferrable to other va...