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In this study, a unique 0-D/2-D Ti3C2 structure was assembled by salt-etching Ti3C2 nanodots out of their parent 2-D Ti3C2 nanosheets. The strong quantum confinement in finite-sized nanodots and concomitant nanodents endowed this structure with a gradient bandgap. UV–Vis diffuse reflectance spectrum revealed the bandgap energies of the coated nanodots and inner nanosheets were 2.82 and 2.40 eV, respectively. Accordingly, the 0-D/2-D Ti3C2 was fairly sensitive to sunlight and could efficiently degrade MB, MeB and RhB dyes in contaminated water under solar illumination. Photocatalytic experiments evidenced that less dye adsorption would induce higher removal ratio of the dye. Moreover, cyclic removal experiments showed the photodegradation efficiency of 0-D/2-D Ti3C2 could still exceed 60% after the fifth cycle for MB, MeB and RhB dyes.