Titanates are one of promising sorbents for toxic heavy metal ions and radionuclides due to various chemical formulas and crystal structures, and their functional properties. Herein, we present a unique seaweed-like sodium titanate mat (SST) with randomly distributed layered sodium dititanate nanofibers synthesized by a simple hydrothermal process. We focused on the effect of NaOH concentration during the hydrothermal process on crystallographic properties and investigated the synthesis conditions for SST. Furthermore, Sr 2+ sorption properties of SST and related titanates, which were synthesized by hydrothermal process, was studied by batch tests. SST, which consist of a dititanate phase, was synthesized at 10 mol/L NaOH concentration and trititanate phase was formed when the NaOH concentration was increased to 15 mol/L. The SST showed a high ionexchange selectivity of Sr 2+ against H + and a high maximum sorption capacity (2 mmol/g), compared with the case of trititanate phase (0.49 mmol/g), which shows the precipitation of SrCO 3 . This was presumably due to the difference of crystal structure of two titanates. This study demonstrates that the design of the crystal structure is important for controlling the sorption mechanism of sorbents for water treatment.