Foam materials saturated with neutron sensitive compounds are of interest as a viable replacement for 3He-based neutron detectors. Previous studies have shown the feasibility of 6LiF-saturated foam detectors as a valid replacement both experimentally and theoretically. However, the random geometry of foam material has previously limited the effective theoretical considerations for such materials to generalized approximations of detector efficiency based on the effective amount of neutron-sensitive material and effective charged-particle ranges. Neutron transport and subsequent charged particle energy deposition have been simulated using novel Monte Carlo methods in order to develop reaction-product pulse-height spectra, to determine intrinsic thermal-neutron detection efficiency, and to optimize material properties for open-cell foam neutron detectors. The theoretical maximum intrinsic thermal-neutron detection efficiency of a 2-inch diameter, 27.5% 6LiF saturated, open-cell foam neutron detector was found to be 39.48% +/− 0.06% (assuming 100% charge extraction from the bulk foam) using observed material properties. The pulse-height spectra and intrinsic neutron detection efficiencies determined from Monte Carlo simulations have been confirmed by comparison to experimental pulse-height spectra. Intrinsic thermal-neutron detection efficiencies of up to 65.90% +/− 0.08% can be obtained for 2-inch diameter, 27.5% 6LiF saturated, open-cell foam by optimizing the foam strut dimensions.