Polysulfones, such as poly(oxy-1,4-phenylenesulfonyl-1,4-phenyleneoxy-1,4-phenyleneisopropylid-ene-1,4-phenylene), poly(phenylene ether sulfone), poly(phenylene sulfone), and aliphatic polysulfone, poly(bicycloheptene sulfone), were employed as a host resin. N-ethyl-N-hydroxyethyl-4-(4'-nitrophenylazo)phenylamine (Disperse Red 1) acted as a guest molecule and was dispersed in those hosts with a concentration of 5 wt. % to 10 wt.%. Their second harmonic generation properties were characterized and compared. Xijk values obtained varied from 11 pm/V to 21 pm/V. The merits of polysulfones as a host material are good optical clarity, easy film forming, and fairly high glass transition Tg temperature (140 °C to 190 °C). Chemically, compared to polyimides they have good resistance to moisture, i.e., less vulnerable to hydrolysis. It is a good candidate for electro-optical materials.