Hybrid materials in optoelectronic devices can generate new functionality or provide synergistic effects that enhance the properties of each component. Here, high-performance phototransistors with broad spectral responsivity in UV-vis-near-infrared (NIR) regions, using gold nanorods (Au NRs)-decorated n-type organic semiconductor and N,N′-bis(2-phenylethyl)-perylene-3,4:9,10tetracarboxylic diimide (BPE-PTCDI) nanowires (NWs) are reported. By way of the synergistic effect of the excellent photo-conducting characteristics of single-crystalline BPE-PTCDI NW and the light scattering and localized surface plasmon resonances (LSPR) of Au NRs, the hybrid system provides new photodetectivity in the NIR spectral region. In the UV-vis region, hybrid nanomaterial-based phototransistors exhibit significantly enhanced photo-responsive properties with a photo-responsivity (R) of 7.70 × 10 5 A W −1 and external quantum efficiency (EQE) of 1.42 × 10 8 % at the minimum light intensity of 2.5 µW cm −2 , which are at least tenfold greater than those of pristine BPE-PTCDI NW-based ones and comparable to those of high-performance inorganic material-based devices. While a pristine BPE-PTCDI NW-based photodetector is insensitive to the NIR spectral region, the hybrid NW-based phototransistor shows an R of 10.7 A W −1 and EQE of 1.35 × 10 3 % under 980 nm wavelength-NIR illumination. This work demonstrates a viable approach to high-performance photo-detecting systems with broad spectral responsivity.