The nonlinear optical properties of four Donor2π2Acceptor (D2π2A) type molecular materials were investigated by their light scattering spectra pumped with 1. 064μm pulsed Nd∶YAG laser. The scattering spectra were acquired by an OMA system. The D2π2Amoleculars consist of Phenyl-polyene and pyrazine as two different conjugated bridge ,biscyan as electron acceptor and dimethyl amino as donor. The moleculars can be two types :one is line and the other isΛ shapped. The chromophores in line type has the higher susecptibility for second harmonic generation while the fluorescence induced by twophonon absorption of typeΛ shows higher third-order nonlinear polarizability. It has shown that the Phenyl-polyene as conjugated bridge can improve the efficiency of charge transfer while pyrazine reduces molecular susecptibility.