Recent emerging developments have demonstrated that bismuth ferrite is one of the promising lead-free perovskite materials used in solar energy harvesting devices and photodetectors. This work reports high short-circuit photocurrent densities of ∼1.2 × 10 3 and ∼0.55 × 10 3 μA/cm 2 in a p-type gadolinium-doped BiFeO 3 ceramic with n-type indium tin oxide under 405 nm irradiation and sunlight at 10 2 mW/cm 2 intensity, respectively. Polarization-enhanced photoresponsivity of ∼5.4 × 10 −2 A/W and specific detectivity of ∼1.5 × 10 11 Jones were achieved with response times of ∼1 and ∼10 ms, respectively, at the rising and decaying edges. Enhanced photovoltaic conversion via a prior electric-field poling can be attributed to the p−n junction and the field-modulated Schottky barrier in conjunction with domain nucleation, ordered polar nanoregions, and increased O 2p−Fe 3d orbital hybridization. The network of domain walls and grain boundaries serves as conduction pathways for the photogenerated charge carriers. The improved photocurrent in gadolinium-doped BiFeO 3 opens up an opportunity for using bismuth ferrite materials in self-powered photodetectors. KEYWORDS: (Bi 0.93 Gd 0.07 )FeO 3 , photocurrent, photoresponsivity, photoresponse time, domain wall