Ultrafast, spatial atmospheric atomic layer deposition, which does not involve vacuum steps and is compatible with roll‐to‐roll processing, is used to grow high quality TiO2 blocking layers for organic solar cells. Dense, uniform thin TiO2 films are grown at temperatures as low as 100 °C in only 37 s (~20 nm/min growth rate). Incorporation of these films in P3HT‐PCBM‐based solar cells shows performances comparable with cells made using TiO2 films deposited with much longer processing times and/or higher temperatures. Copyright © 2013 John Wiley & Sons, Ltd.