Chemical and electrochemical lithium intercalation behavior was investigated on Li2CrTi(PO4)(3). Lithium ions with an almost one mole per formula were inserted by the chemical intercalation by n-butyllithium. The structure refinement was done by the Rietveld method for both parent and intercalated materials. The results showed that both materials crystallized in a lower crystal symmetry, R (3) over bar or C2/c, which is different from that previously reported in the literature. The intercalated material exhibited a cathode performance with a plateau at around 2.8 V vs. Li/Li+ upon charging and 2.4 V vs. Li/Li+ upon discharging.