Plastic photovoltaic devices (PVs) were fabricated by spray-depositing copper indium diselenide (CuInSe2) nanocrystals into micrometer-scale groove features patterned into polyethylene terephthalate (PET) substrates. Each groove has sidewall coatings of Al/CdS and Au and performs as an individual solar cell. These PV groove features can be linked electrically in series to achieve high voltages. For example, cascades of up to 15 grooves have been made with open-circuit voltages of up to 5.8 V. On the basis of the groove geometry, the power conversion efficiencies (PCEs) of the devices reached as high as 2.2%. Using the active area and photovoltaic response of devices determined from light-beam-induced current (LBIC) and photoreflectivity measurements gave PCE values as high as 4.4%.