The photoconductive properties of MBB-PPV/C60 composite films fabricated by the physical jet deposition (PJD) technique have been studied on the basis of the photoinduced charge transfer process. Under the photoexcitation, the transverse photoconductivity of the composite films is greatly enhanced by 4 orders of magnitude due to the efficient excitation transfer process from MBB-PPV (as donor) to C60 (as acceptor) occurring at the interface, the separation of charges and the existence of in-layer free carriers. The results indicate that the conjugated polymer/fullerene composite films optimized by an appropriate configuration have potential applications in photoelectric devices and photonic fields.