Combining water-quality data from multiple sources can help counterbalance diminishing resources for stream monitoring in the United States and lead to important regional and national insights that would not otherwise be possible. Individual monitoring organizations understand their own data very well, but issues can arise when their data are combined with data from other organizations that have used different methods for reporting the same common metadata elements. Such use of multi-source data is termed “secondary use”—the use of data beyond the original intent determined by the organization that collected the data. In this study, we surveyed more than 25 million nutrient records collected by 488 organizations in the United States since 1899 to identify major inconsistencies in metadata elements that limit the secondary use of multi-source data. Nearly 14.5 million of these records had missing or ambiguous information for one or more key metadata elements, including (in decreasing order of records affected) sample fraction, chemical form, parameter name, units of measurement, precise numerical value, and remark codes. As a result, metadata harmonization to make secondary use of these multi-source data will be time consuming, expensive, and inexact. Different data users may make different assumptions about the same ambiguous data, potentially resulting in different conclusions about important environmental issues. The value of these ambiguous data is estimated at \$US12 billion, a substantial collective investment by water-resource organizations in the United States. By comparison, the value of unambiguous data is estimated at \$US8.2 billion. The ambiguous data could be preserved for uses beyond the original intent by developing and implementing standardized metadata practices for future and legacy water-quality data throughout the United States.