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A new neutron SIMulation program based on the versatile GEANT4 toolkit, neuSIM4, has been developed to describe interactions of neutrons in the NE213 liquid scintillator from 0.1 to 3000 MeV. neuSIM4 is designed to accommodate complicated modern detector geometry setups with multiple scintillator detectors, each of which can be outfitted with more than one photo-multiplier. To address a broad spectrum of neutron energies, two new neutron interaction physics models, KSCIN and NxQMD, have been implemented in GEANT4. For neutrons with energy below 110 MeV, we incorporate a total of eleven neutron induced reaction channels on hydrogen and carbon nuclei, including nine carbon inelastic reaction channels, into KSCIN. Beyond 110 MeV, we implement a neutron induced reaction model, NxQMD, in GEANT4. We use its results as reference to evaluate other neutron-interaction physics models in GEANT4. We find that results from an existing cascade physics model (INCL) in GEANT4 agree very well with the results from NxQMD, and results from both codes agree with new and existing light response data. To connect KSCIN to NxQMD or INCL, we introduce a transition region where the contribution of neuSIM4 linearly decreases with corresponding increased contributions from NxQMD or INCL. To demonstrate the application of the new code, we simulate the light response and performance of a 2 × 2 m2 neutron detector wall array consisting of 25 2m-long scintillation bars. We are able to compare the predicted light response functions to the shape of the experimental response functions and calculate the efficiency of the neutron detector array for neutron energies up to 200 MeV. These simulation results will be pivotal for understanding the performance of modern neutron arrays with intricate geometries, especially in the measurements of neutron energy spectra in heavy-ion reactions.