In this study, the design and development of a portable neutron detection system based on a 6LiF + ZnS(Ag) scintillator was carried out. The detector system was first modeled using the Monte Carlo simulation code MCNP. As a result of the detector simulation, the materials and photomultiplier tubes (PMTs) were supplied for the system, and the material properties and thicknesses were optimized for the best scintillator, with the EJ-420 (Eljen Technology), consisting of 95% 6Li dispersed in ZnS(Ag), chosen because it has a distinctive feature with regard to high thermal neutron detection efficiency. Since this material has been shown to offer a significant advantage in favor of neutron detection in mixed radiation fields with gammas and neutrons, the pulse shape discrimination method was employed. To achieve this, a proper electronic circuit was developed to discriminate the pulses from neutrons and gammas. In the experimental step, the EJ-420 scintillator with a 50-mm diameter was optically coupled with a special fast PMT (Hamamatsu H1949-51 model). In conclusion, this study, which underlines the performed simulations for a neutron detector configuration, gives the obtained experimental results showing discrimination capability in neutron/gamma detection using a 241Am-Be neutron source. The results show that the EJ-420 is a good scintillator due to its highly enriched 6Li transmator, which results in more effective neutron measurements when a portable neutron detector design is chosen.