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BiVO4 is widely used in photodegradation and photocatalytic oxygen evolution under visible-light irradiation. In this study, to reduce the recombination rate of photoexcited electrons and holes and increase the reaction activity site, BiVO4–Bi2O3 heterostructural flowers were fabricated by one-pot hydrothermal method by adjusting the concentration of hydrogen ions. Moreover, we used sucrose to control the morphology structure of BiVO4 and form the BiVO4–Bi2O3 heterostructural flowers. The BiVO4–Bi2O3 heterostructural flowers exhibited a higher photodegradation rate of organic pollutant than product synthesized without sucrose, BiVO4, and Bi2O3. The synergistic effect between BiVO4 and Bi2O3 and the recombination frequency of photoexcited electrons and holes as influence factors of improving the photooxidative capability were widely explored. The flower-like morphology provided active sites, and the nanosheets of the flowers decreased the transport distance of the photoexcited carriers.