Laser-induced breakdown spectroscopy (LIBS) is widely dependent on the conditions of its implementation in terms of laser characteristics (wavelength, energy, and pulse duration), focusing conditions, and surrounding gas. In this study two wavelengths, 1.06 and 2.94 microm, obtained with Nd:YAG and Er:YAG lasers, respectively, were used for LIBS analysis of aluminum alloy samples in two conditions of surrounding gas. The influence of the laser wavelength on the laser-produced plasma was studied for the same irradiance by use of air or helium as a buffer gas at atmospheric pressure. We used measurements of light emission to determine the temporally resolved space-averaged electron density and plasma temperature in the laser-induced plasma. We also examined the effect of laser wavelength in two different ambient conditions in terms of spectrochemical analysis by LIBS. The results indicate that the effect of the surrounding gas depends on the laser wavelength and the use of an Er:YAG laser could increase linearity by limiting the leveling in the calibration curve for some elements in aluminum alloys. There is also a significant difference between the plasma induced by the two lasers in terms of electron density and plasma temperature.