Marine aerosol particles play an important role in atmospheric processes. It has been suggested that as marine aerosol particles form, they acquire a coating of organic surfactants. This theory has been supported only by indirect evidence. Recently, we gave new morphological indication of such organic coating without however providing molecular speciation. Here we have studied the surface of marine aerosol particles by time-of-flight secondary ion mass spectrometry (TOF-SIMS), which is very suitable for surface research due to its unique combination of surface sensitivity and the detailed molecular information obtained. Spectra from the outermost surface gave high intensity for palmitic acid and lower peaks for other fatty acids. According to TOF-SIMS images, palmitic acid was distributed on small particles, similar with the marine particles. Sputtering stripped palmitic acid and revealed the inner core of the sea-salt particles. Our results show that fatty acids are important ingredients of the outermost surface layer of the studied aerosol particles.