As with science, so with security in both arenas, the extraordinary sensitivity of cryogenic sensors enables high-confidence detection and high-precision measurement even of the faintest signals. Science applications are more mature, but several national and international security applications have been identified where cryogenic detectors have high potential payoff. International safeguards and nuclear forensics are areas needing new technology and methods to boost speed, sensitivity, precision and accuracy. Successfully applied, improved nuclear materials analysis will help constrain nuclear materials diversion pathways and contribute to treaty verification. Cryogenic microcalorimeter detectors for X-ray, gamma-ray, neutron, and alpha-particle spectrometry are under development with these aims in mind. In each case the unsurpassed energy resolution of microcalorimeters reveals previously invisible spectral features of nuclear materials. Preliminary results of quantitative analysis indicate substantial improvements are still possible, but significant work will be required to fully understand the ultimate performance limits.