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Presented in this paper are the results of an experimental study on the laser induced plasma emission of a number of CN free samples (urea, sucrose) with 40 mJ pulse energy using He and N2 ambient gases. It is shown that the CN emission has its exclusive sources in the molecules produced as the result of chemical bonding either between the ablated C and N ions in the He plasma or between the ablated C and dissociated N from the N2 ambient gas. The emission intensities in both cases are found to have the highest values at the low gas pressure of 2 kPa. The emission in He gas is shown to exhibit the typical characteristics related to a shockwave generated excitation mechanism. The experiments using He ambient gas further demonstrate the feasible laser-induced breakdown spectroscopy application to quantitative and sensitive N analysis of coal and promising application for practical in situ carbon dating of fossils.