Abstract:A new series of non linear optical (NLO) copolyesters have been synthesized by solution polycondensation method. The two diols namely 2,6 bis(4-methoxy-3-hydroxybenzylidene)-3-methylcyclohexanone and 1-(3-hydroxyphenyl)-3-(4-methoxy-3-hydroxyphenyl)-prop-2-en-1-one, isopthaloyl chloride and succinyl, oxalyl and glutaryl chlorides were employed in the synthesis of the six copolyesters. Claisen-Schmidt condensation reaction was employed in synthesizing these two monomer diols. The formed polymeric materials were characterized by involving viscosity measurements, solubility study and FT-IR, 1 H NMR, 13 C NMR and UV-Visible spectroscopic techniques. Thermal transitions of these six copolyesters were recorded in an inert nitrogen atmosphere using Thermogravimetric Analysis. The second harmonic generation (SHG) efficiency of these copolyesters was measured by the standard powder technique using Nd-YAG laser and they were found to be NLO active.