Double slot-die coating using aqueous inks was employed for the simultaneous coating of the active layer and the hole transport layer (HTL) in fully roll-to-roll (R2R) processed polymer solar cells. The double layer film was coated directly onto an electron transport layer (ETL) comprising doped zinc oxide that was processed by single slot-die coating from water. The active layer comprised poly-3-hexylthiophene:Phenyl-C-61-butyric acid methyl ester (P3HT:PCBM) as a dispersion of nanoparticles with a radius of 46 nm in water characterized using small-angle X-ray scattering (SAXS), transmission electron microscopy (TEM), and atomic force microscopy (AFM). The HTL was a dispersion of poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS) in water. The films were analyzed using time-of-flight secondary ion mass spectrometry (TOF-SIMS) as chemical probe and X-ray reflectometry as physical probe, confirming the identity of the layered structure. The devices were completed with a back electrode of either Cu tape or evaporated Ag. Under standard solar spectrum irradiation (AM 1.5G), current-voltage characterization (J-V) yielded an open-circuit voltage (V-oc), short-circuit current (J(sc)), fill factor (FF), and power conversion efficiency (PCE) of 0.24 V, 0.5 mA cm(-2), 25%, and 0.03%, respectively, for the best double slot-die coated cell. A single slot-die coated cell using the same aqueous inks and device architecture yielded a V-oc, J(sc), FF, and PCE of 0.45 V. 1.95 mA cm(-2), 33.1%, and 0.29%, respectively. (C) 2011 Elsevier B.V. All rights reserved.