The article has proved preliminarily connection of dipole moments and frequency doubling effects of organic conjugate molecules. The molecular dipole moments of 3-methyl and 2-tmethyl-4-nitropyridine-l-oxide (3-POM and 2-POM) and 2-halogea and 3-halogen-4-nitroniline (2-CNA, 3-CNA, 2-BNA and 3r-BNA) have been calculated by using EHMO method, and synthesized, their frequency doubling properties and dipole moments have been measured. The experimental results are in agreement with the theoretical production.