Odyssey, one of the NASA’s Mars exploration program and SELENE (Kaguya), a Japanese lunar orbiting spacecraft have a payload of Gamma-Ray Spectrometer (GRS) for analyzing radioactive chemical elements of the atmosphere and the surface. In these days, gamma-ray spectroscopy with a High-Purity Germanium (HPGe) detector has been widely used for the activity measurements of natural radionuclides contained in the soil of the Earth. The energy spectra obtained by the HPGe detectors have been generally analyzed by means of the Window Analysis (WA) method. In this method, activity concentrations are determined by using the net counts of energy window around individual peaks. Meanwhile, an alternative method, the so-called Full Spectrum Analysis (FSA) method uses count numbers not only from full-absorption peaks but from the contributions of Compton scattering due to gamma-rays. Consequently, while it takes a substantial time to obtain a statistically significant result in the WA method, the FSA method requires a much shorter time to reach the same level of the statistical significance. This study shows the validation results of FSA method. We have compared the concentration of radioactivity of 40K, 232Th and 238U in the soil measured by the WA method and the FSA method, respectively. The gamma-ray spectrum of reference materials (RGU and RGTh, KCl) and soil samples were measured by the 120% HPGe detector with cosmic muon veto detector. According to the comparison result of activity concentrations between the FSA and the WA, we could conclude that FSA method is validated against the WA method. This study implies that the FSA method can be used in a harsh measurement environment, such as the gamma-ray measurement in the Moon, in which the level of statistical significance is usually required in a much shorter data acquisition time than the WA method.