A morphology-controlled facile synthesis of titanium-glycolate precursors with subsequent annealing in He and air atmospheres has been exploited for the production of nanostructured composite globules, whiskers and plates of C-modified titanium dioxide. Characterisation tests proved the as-obtained globule composites to exclusively exhibit high-specific surface area (up to 150-170 m 2 g −1), thus being useful for photocatalytic applications in the visible-light region. The combination of the electron paramagnetic resonance, X-ray photoelectron spectroscopy, absorption spectroscopy and transmission electron microscopy revealed the presence of three kinds of carbon in the globules: a small bandgap (with measured width of 0.8 eV) amorphous carbon surrounding the anatase nanocrystallites, C-containing radicals including carbonates on the surface of TiO 2 and interstitial carbon in the oxygen position of the TiO 2 lattice. It was found that the maximum visible-light photocatalytic activity of the globules is determined by the optimal surface concentration of amorphous carbon of about 0.002 wt.% m −2. Under these conditions, the highest synergic photosensitising effect on TiO 2 nanocrystallites of all three kinds of carbon is expected.