High-performance CO2 sorbents typically contain both alkaline compounds and inert supporting materials. The convention is broken by TiO(OH)2. The CO2 sorption capacity of nanostructured TiO(OH)2 reaches 6.1 mmol g-1, while its CO2 sorption selectivity for CO2/N2 mixtures is much higher than that of state-of-the-art sorbents, activated carbon and zeolite, which is another surprise.