A study of the chemical evolution and paragenesis of the uranium minerals at the Palermo No. 1 and Ruggles granitic pegmatites, Grafton County, New Hampshire, revealed four stages of secondary mineralization. A total of eight uranium minerals were identified in the four stages. The first stage is a mixture of uranyl oxide hydroxide-hydrates represented by mineral "A", which surrounds and replaces a uraninite core. The second stage is a carbonate stage found only at the Palermo No. 1 pegmatite, and is represented by rutherfordine. The third stage is represented by uranyl silicates. At the Palermo No. 1 pegmatite, this stage consists of ??-uranophane, and at the Ruggles pegmatite, it consists of soddyite and ??-uranophane. A final fourth stage is a phosphate stage represented by phosphuranylite and meta-autunite I. The first three stages of mineralization developed from hydrothermal and meteoric processes. With dropping temperatures, hydrothermal fluids reached meteoric temperatures and acquired the characteristics of meteoric water. The pH shifted from acidic (pH less than about 6 at 100??C) to alkaline (pH > 7 at 25??C). Since mineral "A" contains hydroxyl and a low amount of molecular water, it probably formed at a temperature greater than 100??C in the acidic environment. After the first stage, the hydrothermal fluids likely reached the temperatures of meteoric water. The initial pH of the meteoric water was acidic (pH less than about 6 at 25??C) and then slowly shifted to alkaline. The mineralizing fluids became oversaturated in CO3, Ca, K, and Si. Uraninite and mineral "A" became unstable and were replaced by rutherfordine and uranyl silicates. The fourth or phosphate stage developed from the introduction of groundwater. The uranyl phosphate minerals precipitated from an acidic fluid (pH < 7 at 25??C) that was oversaturated with Ca, K, U, and P.