Nuclear forensics plays a critical role in national and international security strategies. Advanced technical nuclear forensic capabilities act as a powerful deterrent to nuclear security issues such as nuclear smuggling, nuclear terrorism, nuclear extortion, and nuclear arms proliferation. Source attribution of illicit material can aid in law enforcement actions and promotes materials accountability. The work presented in this dissertation supports the advancement of nuclear forensic capabilities in three ways. The first is through the evaluation of signatures related to nuclear materials. Rare earth element signatures in uranium materials were evaluated in an aqueous environment to assess the influence of environmental aging. The second is through the development of a surrogate nuclear melt glass that can be used as a reference material during the in situ analysis of nuclear debris materials. An urban melt glass containing aluminum, calcium, strontium, lanthanum, gadolinium, and uranium was synthesized using a sol-gel technique and determined to be homogeneous at the microscale. Finally, the rapid decomposition of glassy matrices, representative of nuclear melt glass, was investigated via nitrogen trifluoride fluorination.