Abstract: The neutron sensitivity of a cylindrical circle minus 1.5 in x 1.5 in LaBr3:Ce scintillation detector was measured using quasi-monoenergetic neutron beams in the energy range from 40 keV to 2.5 MeV. In this energy range the detector is sensitive to gamma-rays generated in neutron inelastic and capture processes. The experimental energy response was compared with Monte Carlo simulations performed with the Geant4 simulation toolkit using the so-called High Precision Neutron Models. These models rely on relevant information stored in evaluated nuclear data libraries. The performance of the Geant4 Neutron Data Library as well as several standard nuclear data libraries was investigated. In the latter case this was made possible by the use of a conversion tool that allowed the direct use of the data from other libraries in Geant4. Overall it was found that there was good agreement with experiment for some of the neutron data bases like ENDF/B-VII.0 or JENDL-3.3 but not with the others such as ENDF/B-VI.8 or JEFF-3.1.