Abstract: An improved lithium secondary battery using a novel layered titanium phosphate having the formula of TiO(OH)(H.sub.2 PO.sub.4), or LTP, as anode material, and LiCoO.sub.2, LiNiO.sub.2, or other appropriate material, as cathode. A stable operating voltage of 3-volt can be obtained from the resultant lithium secondary battery. The layered titanium phosphate is prepared by first reacting a tetramethylammonium hydroxide (N(CH.sub.3).sub.4 OH) solution containing orthophosphoric acid with titanium dioxide in a low temperature hydrothermal reaction to form a tetramethylammonium form of layered titanium phosphate, or NMe.sub.4 TP, which serves as the precursor of LTP. The precursor NMe.sub.4 TP is then placed in a concentrated hydrochloric acid at room temperature to obtain a high purity LTP via a cation exchange reaction. Each of the Li.sub.