The present research was planned to develop a method for species concentration measurements under high temperature and pressure environments. The characteristics of CO2 spectrum at high temperature and pressure were studied at first. Based on the research above, tunable diode-laser absorption of CO2 near 2.0 μm incorporating fixed-wavelength modulation spectroscopy with second-harmonic detection was used to provide a method for sensitive and accurate measurements of gas temperature and CO2 concentration at high temperature and pressure. Measurements were performed in a well-controlled high temperature and pressure static cell. The results show that the average error of the CO2 concentration measurements at 5 atm, 500 K and 10 atm, 1000 K is 4.49%. All measurements show the accuracy and potential utility of the method for high temperature and pressure diagnostics.