The subcritical multiplication factor is considered an important index for recognizing, in the core, the number of fission neutrons induced by an external neutron source. In this study, the influences of different external neutron sources on core characteristics are carefully monitored. Here, the high-energy neutrons generated by the neutron yield at the location of the target are attained by the injection of 100 MeV protons onto these targets. In actual ADS cores, liquid Pb–Bi has been selected as a material for the target that generates spallation neutrons and for the coolant in fast neutron spectrum cores. The neutron spectrum information is acquired by the foil activation method in the 235U-fueled and Pb–Bi-zoned fuel region of the core, modeling the Pb–Bi coolant core locally around the central region. The neutron spectrum is considered an important parameter for recognizing information on neutron energy at the target. Also, the neutron spectrum evaluated by reliable methodologies could contribute to the accurate prediction of reactor physics parameters in the core through numerical simulations of desired precision. In the present chapter, experimental analyses of high-energy neutrons over 20 MeV are conducted after adequate preparation of experimental settings.