The energy spectra of neutrons were measured by a time-of-flight method for 120GeV protons on thick graphite, aluminum, copper, and tungsten targets with an NE213 scintillator at the Fermilab Test Beam Facility. Neutron energy spectra were obtained between 25 and 3000MeV at emission angles of 30°, 45°, 120°, and 150°. The spectra were parameterized as neutron emissions from three moving sources and then compared with theoretical spectra calculated by PHITS and FLUKA codes. The yields of the theoretical spectra were substantially underestimated compared with the yields of measured spectra. The integrated neutron yields from 25 to 3000MeV calculated with PHITS code were 16–36% of the experimental yields and those calculated with FLUKA code were 26–57% of the experimental yields for all targets and emission angles.