A Monte Carlo simulation-based optimization of a SERS-based thermal neutron detector is aimed at improving detection efficiency for thermal neutrons. The moderator and collimator have been designed for a 241Am-9Be source to maximize the thermal neutrons flux in the irradiation area. Simulated thermal neutron detection efficiency can be increased to approximately 50.5% when polyethylene is added as neutron reflector and 10B enriched 4-MPBA is used. With Monte Carlo software GEANT4, the SERS-based thermal neutron detector has been proven to have almost no effect on original thermal neutron flux as well as the distribution and could be used for thermal neutron detection accurately.