The National Land Cover Database (NLCD) provides time-series data characterizing the land surface for the United States, including land cover and tree canopy cover (NLCD-TC). NLCD-TC was first published for 2001, followed by versions for 2011 (released in 2016) and 2011 and 2016 (released in 2019). As the only nationwide tree canopy layer, there is value in assessing NLCD-TC accuracy, given the need for cross-city comparisons of urban forest characteristics. Accuracy assessments have only been conducted for the 2001 data and suggest substantial inaccuracies for that dataset in cities. For the most recent NLCD-TC version, we used various datasets that characterize the built environment, weather, and climate to assess their accuracy in different contexts within 27 cities. Overall, NLCD underestimates tree canopy in urban areas by 9.9% when compared to estimates derived from those high-resolution datasets. Underestimation is greater in higher-density urban areas (13.9%) than in suburban areas (11.0%) and undeveloped areas (6.4%). To evaluate how NLCD-TC error in cities could be reduced, we developed a decision tree model that uses various remotely sensed and built-environment datasets such as building footprints, urban morphology types, NDVI (Normalized Difference Vegetation Index), and surface temperature as explanatory variables. This predictive model removes bias and improves the accuracy of NLCD-TC by about 3%. Finally, we show the potential applications of improved urban tree cover data through the examples of ecosystem accounting in Seattle, WA, and Denver, CO. The outputs of rainfall interception and urban heat mitigation models were highly sensitive to the choice of tree cover input data. Corrected data brought results closer to those from high-resolution model runs in all cases, with some variation by city, model, and ecosystem type. This suggests paths forward for improving the quality of urban environmental models that require tree canopy data as a key model input.