The Niwot Ridge and Green Lakes Valley (NWT) long-term ecological research (LTER) site collects environmental observations spanning both alpine and subalpine regimes. The first observations began in 1952 and have since expanded to nearly 300 available datasets over an area of 99 km2 within the north-central Colorado Rocky Mountains that include hydrological (n = 101), biological (n = 79), biogeochemical (n = 62), and geographical (n = 56) observations. The NWT LTER database is well suited to support hydrologic investigations that require long-term and interdisciplinary data sets. Experimentation and data collection at the NWT LTER are designed to characterize ecological responses of high-mountain environments to changes in climate, nutrients, and water availability. In addition to the continuation of the many legacy NWT datasets, expansion of the breadth and utility of the NWT LTER database is driven by new initiatives including (a) a catchment-scale sensor network of soil moisture, temperature, humidity, and snow-depth observations to understand hydrologic connectivity and (b) snow-albedo alteration experiments using black carbon to evaluate the effects of snow-disappearance on ecosystems. Together, these observational and experimental datasets provide a substantial foundation for hydrologic studies seeking to understand and predict changes to catchment and local-scale process interactions.