Near‐surface air quality (AQ) observations over coastal waters are scarce, a situation that limits our capacity to monitor pollution events at land‐water interfaces. Satellite measurements of total column (TC) nitrogen dioxide (NO2) observations are a useful proxy for combustion sources, but the once daily snapshots available from most sensors are insufficient for tracking the diurnal evolution and transport of pollution. Ground‐based remote sensors like the Pandora Spectrometer Instrument (PSI) that have been developed to verify space‐based TC NO2 and other trace gases are being tested for routine use as certified AQ monitors. The KORUS‐OC (Korea‐United States Ocean Color) cruise aboard the R/V Onnuri in May–June 2016 represented an opportunity to study AQ near the South Korean coast, a region affected by both local/regional and long‐distance pollution sources. Using PSI data in direct‐Sun mode and in situ sensors for shipboard ozone, CO, and NO2, we explore, for the first time, relationships between TC NO2 and surface AQ in this coastal region. Three case studies illustrate the value of the PSI and complexities in the surface‐column NO2 relationship caused by varying meteorological conditions. Case Study 1 (25–26 May 2016) exhibited a high correlation of surface NO2 to TC NO2 measured by both PSI and Aura's Ozone Monitoring Instrument, but two other cases displayed poor relationships between in situ and TC NO2 due to decoupling of pollution layers from the surface. With suitable interpretation the PSI TC NO2 measurement demonstrates good potential for working with upcoming geostationary satellites to advance diurnal tracking of pollution.