Anatase TiO(2) nanocuboids wholly exposed with high-energy {001} and {100} facets were successfully synthesized by a novel, environmentally benign synthetic strategy using acid-delaminated vermiculite (DVMT) and tetramethylammonium hydroxide as synergistic morphology-controlling reagents, where the DVMT layers act as effective hard template selectively stabilizing the {001} facets of TiO(2).