Two condensed phthalazine compounds were synthesized and characterized by FT-IR, UV-Vis, NMR spectroscopic studies. Single crystal XRD and molecular orbital calculations. Optimized geometrical structures were computed with RB3LYP method with the 6-31G(p, d) basis set. The geometrical parameters of both compounds obtained from Single Crystal XRD were found to be in accord with the calculated (DFT) values. The electronic contribution χ <3> T HG was measured using the third harmonic generation technique on thin films at 1064 nm for both compounds. Also, the values of dipole moment μ, the average polarizabilityᾱ, and the first static hyperpolarizability (β 0) were computed. The theoretical and experimental results confirm the NLO behavior of both compounds.