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In order to realize high efficiency visible-light absorption and electron–hole separation of bismuth vanadate (BVO), we synthesized carbon-doped BVO (C-BVO) with high visible-light absorption behavior. We used polyvinylpyrrolidone K-30 as a template and l-cysteine as the carbon source in a one-step hydrothermal synthesis method, and then obtained the carbon-doped BVO@multi-walled carbon nanotubes (C-BVO@MWCNT) by a two-step method. The carbon nanotubes were characterized by X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy, UV-vis diffuse reflectance spectroscopy, specific surface area, electron spin resonance, and transient photocurrent responses. The XRD analysis confirmed that all photocatalysts were in the same crystal form with a single monoclinic scheelite structure. Combining this with the other characterization results, we showed that the carbon element was successfully doped in BVO and the resulting C-BVO was successfully coupled with multi-walled carbon nanotubes. The removal ratio of rhodamine B by C-BVO@MWCNT was much higher than those by BVO and C-BVO under visible-light irradiation. Recycling experiments verified the stability of C-BVO@MWCNT, which was proved to offer excellent adsorption, strong visible-light absorption behavior, and high electron–hole separation efficiency. Such properties are expected to be useful in practical applications. [ABSTRACT FROM AUTHOR]