Neutron radiation detectors are an integral part of the Department of Homeland Security (DHS) efforts to detect the illicit trafficking of radioactive or special nuclear materials into the U.S. In the past decade, the DHS has deployed a vast network of radiation detection systems at various key positions to prevent or to minimize the risk associated with the malevolent use of these materials. The greatest portion of this detection burden has been borne by systems equipped with 3He because of its highly desirable physical and nuclear properties. However, a dramatic increase in demand and dwindling supply, combined with a lack of oversight for the existing 3He stockpile has produced a critical shortage of this gas which has virtually eliminated its viability for detector applications. A number of research efforts have been undertaken to develop suitable 3He replacements; however, these studies have been solely targeted toward simple detection cases where the overall detection efficiency is the only concern. For these cases, an insertion of additional detectors or materials can produce reaction rates that are sufficient, because the neutron spectral response is essentially irrelevant. However, in applications such as safeguards, non-proliferation efforts, and material control and accountability programs (MC&A), a failure to use detectors that are spectrally matched to 3He can potentially produce dire consequences. This is because these more difficult detection scenarios are associated with fissile material assessments for 239Pu and other actinides and these analyses have almost universally been calibrated to an equivalent 3He response. In these instances, a “simple” detector or material addition approach is neither appropriate nor possible, due to influences resulting from the complex nature of neutron scattering in moderators, cross sections, gas pressure variations, geometries, and surrounding structural interference. These more challenging detection cases require a detailed computational transport analysis be performed for each specific application. A leveraged approach using adjoint transport computations that are validated by forward transport and Monte Carlo computations and laboratory measurements can address these more complex detection cases and this methodology was utilized in the execution of the research. The initial task was to establish the fidelity of a computational approach by executing radiation transport models for existing BF3 and 3He tubes and then comparing the modeling results to laboratory measurements made using these identical devices. Both tubes were 19.6 cm in height, 1-inch in diameter, and operated at 1 and 4 atm pressure respectively. The models were processed using a combination of forward Monte Carlo and forward and adjoint 3-D discrete ordinates (SN) transport methods. The computer codes MCNP5 and PENTRAN were used for all calculations of a nickel-shielded plutonium-beryllium (PuBe) source term that provided a neutron output spectra equivalent to that of weapons-grade plutonium (WGPu). Once the computational design approach was validated, the adjoint SN method was used to iteratively identify six distinct plug-in models that matched the neutron spectral response and reaction rate of a 1-inch diameter 3He tube with a length of 10 cm and operating at 4 atm pressure. The equivalent designs consist of large singular tubes and dual tubes containing BF3 gas, 10B linings, and/or 10B-loaded polyvinyl toluene (PVT). The reaction rate for each plug-in design was also verified using forward PENTRAN and MCNP5 calculations. In addition to the equivalent designs, the adjoint method also yielded various insights into neutron detector design that can lead to additional designs using a combination of different detector materials such as BF3/10B-loaded PVT, 10B-lined tubes/10B-loaded PVT, etc.