To obtain the characteristic information of unknown radionuclides by analyzing the γ-energy spectrum of a low-resolution detector, and to improve the accuracy and validity of the analysis of overlapping and weak peaks in the γ-energy spectrum, in this paper we analyze the γ-energy spectrum of NaI(Tl) detectors based on the Boosted-Gold algorithm. A simulation model of NaI(TI) detector is established by using MCNPX, and a detector response matrix with dimension 201 × 200 is obtained. The γ-energy spectrum unfolding program is developed based on the Boosted-Gold algorithm. The detector response spectra of the γ radioactive sources ²²Na, ¹³³Ba, and ¹⁵²Eu are measured. Three groups of low-resolution γ spectra are constructed with different γ-ray energy, different energy differences ( $ \Delta E $ ) and different relative intensities by simulation. Combining the response matrix and the unfolding procedures, the measured and simulated γ energy spectra are unfolded. The unfolding results are analyzed with the nuclide standard characteristics information from the IAEA database. The results show that the maximum unfolding error of the characteristic energy of the measured γ-energy spectrum is 2.17% (0.276 MeV for ¹³³Ba source) by the Boosted-Gold algorithm, and the maximum deviation between the unfolded intensity and the standard intensity is 0.197 (1.408 MeV for ¹⁵²Eu source). For the simulated γ energy spectrum, the characteristic energy of nuclide can be accurately analyzed, and the deviation between unfolded intensity and standard intensity maintains 0.01. When the enhancement factor p≤ 14, the Boosted-Gold algorithm is beneficial to the quantitative analysis of γ-radionuclides. For the relative intensity of γ-rays greater than 10%, this algorithm has better analysis accuracy.