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Based on the Gravel algorithm and the MLEM algorithm, the neutron energy spectrum unfolding algorithms has been developed by using the SY2001 plastic scintillator detector in its entirety to experimentally measure neutron source characterization of the compact D–D neutron generator. In particular, the degree of optimization of the Mean Relative Error (MRE) is proposed as a determinant of the appropriate termination point for iterations to improve the adaptive nature of the algorithm. The developed neutron energy spectrum unfolding algorithms measure the neutron energy spectra and the neutron angular yields of the compact D–D neutron generator, which are compared with Monte Carlo calculated results. Given the good agreement with the existing results, the developed unfolding algorithms can be used to accurately unfolding neutron energy spectrum, especially, for non-pulsed neutron sources. The measured neutron source characterization results show that the compact D–D neutron generator can produce high yields and quasi-mono-energetic neutrons in the range from 2.2 to 2.8 MeV. The D–D neutron angular yields are anisotropic distributions, particularly, which are relatively higher with neutron emission angles ranging from 40 ∘ to 120 ∘ . This work measure the neutron energy spectra and the neutron angular yields of the compact D–D neutron generator in Lanzhou University, which provide detailed neutron source characterization for using it in neutron physics and neutron application technology. [ABSTRACT FROM AUTHOR]