The chemistry of underground storage tanks containing high-level waste at the Hanford Site in Washington State is an area of continued research interest. Thermodynamic models have predicted the formation of analcime and clinoptilolite in Hanford tanks, rather than cancrinite; however, these predictions were based on carbonate-cancrinite. We report the first observation of a nitrate-cancrinite [possibly Na8(K,Cs)(AlSiO4)6(NO3)2 x nH2O] extracted from a Hanford tank 241-AP-101 sample that was evaporated to 6, 8, and 10 M NaOH concentrations. The nitrate-cancrinite phase formed spherical aggregates (4 microm in diameter) that consisted of platy hexagonal crystals (approximately 0.2 microm thick). Cesium-137 was concentrated in these aluminosilicate structures. These phases possessed a morphology identical to that of nitrate-cancrinite synthesized using simulant tests of nonradioactive tank waste, supporting the contention that it is possible to develop nonradioactive artificial sludges. This investigation points to the continued importance of understanding the solubility of NO3-cancrinite and related phases. Knowledge of the detailed structure of actual phases in the tank waste helps with thermodynamic modeling of tank conditions and waste processing.