The hydrothermal preparation of flower-like layered sodium titanate architectures in a weakly alkaline medium is reported. NaCl was used as a morphology-directing agent, and a growth mechanism was proposed. The hierarchical structure is assembled from one-dimensional nanoribbons and exhibits an excellent removal capacity toward methylene blue (MB). A pseudo-second-order kinetic model was found to well describe the adsorption kinetics. Kinetic studies demonstrated that the overall rate of MB adsorption was controlled by surface adsorption and intraparticle diffusion. Results of this work are of great significance for environmental applications of flower-like layered sodium titanate architectures as a promising adsorbent material used for water purification.