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Single-walled carbon nanotubes (SWNTs) were determined to have significant interaction with poly(3-hexylthiophene) (P3HT), which is helpful to form continuous active film with  interpenetrating structure and improve the crystallinity of the resultant film for SWNTs/P3HT composite.Photovoltaic devices basedon an active film with relatively higher crystallinity display much enhanced performance. The work functionof carbon nanotubes modulated by electron transferring from P3HT to SWNTs is proposed to explain thehigh open-circuit voltage (VOC) obtained from the photovoltaic devices based on the SWNTs/P3HT system.