Microstructure, phase transformation behavior and electrical properties of BaTi1-x(Li2/3Nb2/3)xO3 with x=0.01-0.40 ceramics have been investigated. Only perovskite phase is detected for all the compositions. The room temperature state of BaTi1-x(Li2/3Nb2/3)xO3 ceramics experiences a transformation from a ferroelectric phase to a paraelectric phase with increasing x. Meanwhile, the permittivity of BaTi1-x(Li2/3Nb2/3)xO3 ceramics reduces, while the Q×f value increases. A degree of frequency dispersion of dielectric peak is obviously increased as x increases from 0.01 to 0.10. It is of great interest that a dielectric abnormity represented by a broad dielectric peak at 200-400K is observed for the composition with x=0.40.