Accurate, sensitive, and high-coverage analysis of various organic pollutants in complex samples and single cells is significant in investigating their environmental behaviors and toxic effects. Here we proposed a nanospray laser-induced plasma ionization mass spectrometry (nLIPI-MS) method for sensitive and high-coverage analysis of broad polarity organic pollutants under ambient and open-air conditions. The nLIPI-MS method combines nanospray with laser-induced plasma ionization, enabling direct analysis without sophisticated sample pretreatment. For the analysis of nonpolar and very weakly polar organic pollutants such as polycyclic aromatic hydrocarbons (PAHs) and alkyl-PAHs, the nLIPI-MS method showed desirable analytical performance, with limits of detection of as low as the μg/L level. For moderately polar organic pollutants such as