© The Royal Society of Chemistry. The synthesis of titanophosphate nanosheets in aqueous sols was examined by the bottom-up process. The nanosheets were formed by mixing titanium iso-propoxide, phosphoric acid, and tetraalkylammonium hydroxide (NR4OH) aqueous solutions, followed by diluting with water and heating at 80 °C, forming translucent aqueous sols of titanophosphate nanosheets with the same crystal structure as layered titanium phosphate Ti2O3(H2PO4)2·2H2O. Whether the nanosheets were crystallized depended on the reactions during the mixing of reagents before the water dilution. By controlling the acid-base reactions between the Ti species, phosphoric acid, and the hydroxides of bulky cations in the aqueous sols, the one-pot process yielded highly water-dispersible, flake-like titanophosphate nanosheets. Under some synthetic conditions, nanosheets formed even in weakly basic aqueous sols. These nanosheets can be coated on a substrate with low alkali-resistance, or used for the removal of metal ions from neutral aqueous solutions.