H+-restacked nanosheets and nanoscrolls peeled from K4Nb6O17 display different structures and surface characters. The two restacked samples with increased surface areas have an amazing visible-light response for the photodegradation of dyes, which is superior to commercial TiO2 (P25) and Nb205. By comparison, H+/nanosheets have a relatively faster photodegradation rate originated from large and smooth basal plane. The work reveals that dye adsorbed on the unfolded nanosheets can effectively harvest sunlight. Due to facile preparation, low-cost and high photocatalytic efficiency, H+/nanosheets and H+/nanoscrolls might be used for the visible light-driven degradation of organic dyes as a substitute for TiO2 in industry.