This paper presents the results of an experiment determining (n,2n), (n,p), (n,pn), (n,α), (n,n’γ), and (n,γ) reaction rates in 15 test samples of both natural and high-enriched composition: natMg, 27Al, natTi, natFe, 59Co, natNi, 63Сu (99.5%), 65Cu (99.7%), 64Zn (99.4%), natZr, 93Nb, natCd, natIn, 169Tm, and 197Au. Computer simulations in the NG-24M neutron generator spectrum were carried out using the MCNP5 and KIR2 radiation transport codes with different nuclear data libraries (JEFF-3.2, JEFF-3.3, JENDL-4.0, ENDF/B-VII.0, ENDF/B-VII.1, ENDF/B-VIII.0, ROSFOND-2010, FENDL-3.0, TENDL-2019, and IRDFFII). The elaborated full-scale model for neutron transport analysis included the geometry and composition of the neutron generator, experimental samples, and laboratory room. The mean square deviation factor was used to compare the experimental and the simulated results. The best predictive results for both the MCNP5 code and the KIR2 code were obtained with the FENDL-3.0 and ENDF/B-VIII.0 libraries.