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Lithium salt of substituted nanotube is suggested as a new kind of nonlinear optical (NLO) material. It is
found that the combination of the lithiation effect and the donor substitution effect can greatly enhance
the static first hyperpolarizability (b0). Specially, the unusual donor – acceptor(nanotube) – donor system
Li–NT(6,0)–(NH2)2 has considerable b0 to be 6.8  105 au, due to its small transition energy and large
transition moment. Further, the relationships between b0 and the number of Li atoms m and the substituents
R for Lim–NT(6,0)–(R)2 (m = 1, 6 and R = –CN, –NH2) systems are explored.