The invention provides a gamma ray spectra spectrum unfolding method and device for element capture spectrometry logging. The spectrum unfolding method comprises the steps that first, data obtained byan element capture spectrometry logger are preprocessed; then through the theoretical analysis and numerical calculation of spectral shapes, characteristic peak tracks, and backgrounds of different elements, and a main element group and an auxiliary element group are constructed according to the degree of interaction between the elements; then the least square method is used for unfolding the spectrum based on the construction of the main element group and the auxiliary element group; and finally, the yield of each element obtained by the least square method is reconstructed by theory, and the measured gamma ray spectrum and the reconstructed gamma ray spectrum are compared for error control to improve the accuracy of spectral unfolding. The spectrum unfolding method has the advantages ofhigh accuracy and high operability, has good universality for different types of reservoirs, and at the same time, an important reference significance for processing of neutron gamma ray spectrum data of other types of instruments is provided.