It has been demonstrated that a spectrochemical analysis of carbon using the laser plasma method can be successfully applied to inspect the carbonation of concrete by detecting carbon produced in aged concrete by a chemical reaction of Ca(OH)2 with CO2 gas in environmental air, turning into CaCO3, which induces degradation of the quality of building concrete. A comparative study has been made using a TEA CO2 laser (500-1000 mJ) and a Q-switched Nd-YAG laser (50-200 mJ) to search for the optimum conditions for carbon analysis, proving the advantage of the TEA CO2 laser for this purpose. Also, it was clarified that laser irradiation with suitable defocusing conditions is a crucial point for obtaining high sensitivity in the detection of carbon. Practical experiments on the inspection of carbonation were carried out using both a concrete sample that had been intentionally carbonated by exposure to high concentrations of CO2 gas and a naturally carbonated concrete sample. As a result, good coincidence was observed between the laser method and the ordinary method, which uses the chemical indicator phenolphthalein, implying that this laser technique is applicable as an in situ quantitative method of inspection for carbonation of concrete.