Nanospray desorption electrospray ionization (nano-DESI) combined with high-resolution mass spectrometry (HR-MS) is a promising approach for the detailed, molecular-level chemical characterization of atmospheric organic aerosols (OA) collected in laboratory and field experiments. The nano-DESI technique possesses distinct advantages of technical simplicity, enhanced sensitivity, and signal stability. In nano-DESI, analyte is desorbed into a solvent bridge formed between two capillaries and the analysis surface, which enables fast and efficient characterization of OA collected on substrates without sample preparation. Stable signals achieved using nano-DESI make it possible to obtain high-quality HR-MS data both for laboratory-generated and field-collected OA using only a small amount of material (<10 ng). Furthermore, nano-DESI enables the efficient detection of chemically labile compounds in OA, which is important for understanding chemical aging phenomena.