Lithium-containing molecules, such as C 2 H 2 Li 2 , C 6 Li 6 , and several lithium halides, have been studied in the present paper, and the nature of lithium bonds in these structures is investigated. In contrast to the hydrogen bond, which features a typical quasi-linear and dicoordinated (X•••H−Y) geometry, the ionic lithium bond prefers nonlinear and multicoodinated geometrical arrangements. On the basis of these observations, we have predicted some novel energetically low-lying C 6 Li 6 structures. With its unusual features, the Li bond theory should be applied rather widely.