The effect of exposing cyanine–fullerene C60 bilayer solar cells to ambient atmosphere is investigated. For exposure times of a few hours and concomitant light soaking, the device performance experiences a drastic power efficiency increase going from 0.14% to 1.2% measured at 30 mW/cm2 simulated solar irradiation. The 10-fold enhancement is attributed to the photoinduced doping involving oxygen and water leading to the formation of reactive superoxide anions and mobile holes in the cyanine layer. The influence of water and dry oxygen are investigated separately. While water deteriorates the device performance, dry oxygen leads only to a partial increase of efficiency. Annealing does not ameliorate the performance of doped devices. Although then the cyanine layer features more crystallinity, the considerable morphological changes cause diffusional loss in charge carrier collection. Doping of not annealed devices brings a sizeable efficiency enhancement that highlights the importance of charge carrier transport in cyanine dye based solar cells.