Because carbon nanotube (CNT) films have high photothermal conversion efficiency (PTCE), they have been widely used in bolometric and photothermoelectric photodetectors, seawater desalination, and cancer therapy. Here, we present a simple, quick, and non-destructive method to measure the PTCE of CNT films. According to the linear relationship between the Raman shift of the G+ peak and the temperature of a CNT, the offset of the G+ peak under varying excitation light power can characterize the changed temperature. Combining the simulation of the temperature distribution, the final value of the PTCE can be obtained. Finally, a CNT film with a high PTCE was chosen to be fabricated as a bolometric photodetector; a quite high responsivity (2 A W−1 at 532 nm) of this device demonstrated the effectiveness of our method.