The performance of photoresponsive organic FETs (photOFETs) intimately depends on their optical absorption and charge carrier transport property. We report on red light responsive photOFETs based on various device structures utilizing neodymium phthalocyanine (NdPc2) as the light sensitive material. PhotOFETs based on planar heterojunction, bulk heterojunction (BHJ), and hybrid planar–BHJ (HPBHJ) with NdPc2 and C60 on poly(vinyl alcohol) (PVA) and SiO2 gate dielectric were fabricated and characterized. Among various device structures, HPBHJ-photOFET on PVA dielectric showed the best performance. For the 650-nm-red light illumination, an ultrahigh photoresponsivity of 108 A/W and a maximum photosensitivity of $3.75 \times 10^{4}$ were obtained. The ultrahigh enhancement of the photoresponsivity for HPBHJ-photOFET is resulted from high absorption coefficient of NdPc2 in the red light region, high dissociation efficiency of the photogenerated excitons, and high electron mobility of C60 layer grown on PVA.