City-wide air pollution assessments have typically relied on a small number of widely separated regulatory monitoring sites or land use regression (LUR) models built using time-integrated samples to assess annual average population-scale exposure. However, air pollutant concentrations often exhibit significant spatial and temporal variability depending on local sources and features of the built environment. In 2016, the Center for Air, Climate, and Energy Solutions (CACES) Air Quality Observatory was launched at Carnegie Mellon University to better understand urban spatial and temporal pollution gradients on the 8 h) above the regional background. Compared to the non-decomposed total pollutant signal, the short-lived or persistent enhancement pollutant signals, which should come from local sources, were better correlated with covariates used in LUR model construction. For example, Pearson r between total vehicle counts in a 100 m buffer and NO2 increased from 0.57 using the total pollutant signal to 0.83 using the persistent enhancement only. The findings from this study support building more accurate and higher time resolution (e.g., daily, hourly) LURs using low-cost sensors.