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Based on graphene, a new class of second-order nonlinear optical(NLO) material, the lithium salt of NH-substituted graphene nanoribbon with the twofold donor(D)/acceptor(A) mode, was reported. Eight stable 2Li-2NH-GNR lithium salts, especially cis lithium salts, display considerably large β values. The combination of NH-substituting and cis Li-doping makes β greatly increased from O(GNR) to 1.2×10 a.u.(cis-2Li- 2NH-GNRs). Our largest β value(2.9×10 a.u. for a long donor-acceptor polyene.