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This report demonstrates the synthesis of a trihybrid system (PBI-NP-GO) consisting of perylene bisimide appended peptide (PBI-UW) nanofibers, silver nanoparticles (PBI-AgNP), and graphene oxide (GO) nanosheet. Tryptophan-containing PBI molecules in an aqueous medium can reduce silver ions into silver nanoparticles in the presence of sunlight to form a dihybrid system consisting of nanofibers and nanoparticles; the addition of GO into the dihybrid system ultimately leads to the formation of the trihybrid system. The trihybrid system was thoroughly characterized by various spectroscopic and microscopic techniques, such as ultraviolet-visible (UV-vis), Fourier transform-infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), RAMAN, and field emission transmission electron microscopy (FEG-TEM). The so-formed trihybrid system was successfully utilized as a potential photocatalyst for the reduction of carcinogenic Cr(VI) to non-toxic Cr(III) under irradiation with blue LED light. An almost complete reduction of Cr(VI) was achieved within 30 minutes of irradiation. Moreover, good photo-switching behaviour was observed with the highest photocurrent gain of 5.11 (Ion/Ioff) compared to PBI-AgNP (dihybrid) and PBI-UW, where Ion/Ioff values of 3.92 and 2.31, respectively, were obtained. The photocatalytic activity and photo-switching behaviour of the trihybrid system are due to efficient photo-induced charge separation. [ABSTRACT FROM AUTHOR]