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Nitrogen-doped HTiNbO nanosheets have been successfully synthesized by first exfoliating layered HTiNbO in tetrabutylammonium hydroxide (TBAOH) to obtain HTiNbO nanosheets and then heating the nanosheets with urea. The resulting samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), Energy-dispersive X-ray (EDX), X-ray photoelectron spectroscopy (XPS), UV-vis spectroscopy and N adsorption-desorption measurements. It was found that N-doping resulted in a much higher thermostability of the layered structure, intrinsic bandgap narrowing and a visible light response. The doped nitrogen atoms were mainly located in the interstitial sites of TiNbO lamellae and chemically bound to hydrogen ions. Compared with N-doped HTiNbO, N-doped HTiNbO nanosheets had a much larger specific surface area and richer mesoporosity due to the rather loose and irregular arrangement of titanoniobate nanosheets. Both N-doped layered HTiNbO and HTiNbO nanosheets showed a very high visible-light photocatalytic activity for the degradation of rhodamine B (RhB) aqueous solution. Moreover, due to the considerably larger surface area, richer mesoporosity and stronger acidity, N-doped HTiNbO nanosheets had an even higher activity than N-doped HTiNbO, although the latter had a stronger absorption in the visible region. The dye molecules were mainly degraded to aliphatic organic compounds and partially mineralized to CO and/or CO, rather than being simply decolorized. The effect of photosensitization was insignificant and RhB was degraded mainly via the typical photocatalytic reaction routes. Two different reaction routes for the photodegradation of RhB under visible light irradiation over N-doped HTiNbO nanosheets have been proposed. The present method can be extended to a large number of layered metal oxides that have the characteristics of intercalation and exfoliation, thus providing new opportunities for the fabrication of highly effective and potentially practical visible-light photocatalysts. [InlineMediaObject not available: see fulltext.] [ABSTRACT FROM AUTHOR]