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Bismuth vanadate (BiVO4) is a promising photocatalytic material for use in environmental protection and water splitting. However, its short photogenerated carrier lifetime and narrow visible-light response restrict its extensive application. Herein, a novel electrospinning method was developed to prepare bismuth (Bi)-modified BiVO4 (Bi/BiVO4) porous nanofibers. The morphologies, structures, and chemical states of the obtained samples were characterized using a series of analytical techniques. The photocatalytic performance of the Bi/BiVO4 porous nanofibers was evaluated via the photocatalytic degradation of methylene blue (MB) under visible-light irradiation. The enhanced visible-light photocatalytic activity of Bi/BiVO4 can be attributed to the Bi nanoparticles, which exhibit a surface plasmon resonance (SPR) effect and have semiconductor character, extending the optical absorption of BiVO4 and restraining the recombination of electron–hole pairs during the photocatalytic degradation process, respectively. In this work, new insight is provided into the fabrication of a Bi/BiVO4 composite, which can act as an outstanding visible-light responsive photocatalyst, facilitating its application in the field of environmental protection. [ABSTRACT FROM AUTHOR]