The results of air pollution assessment during a 2017 cruise of the research ship “Minerva Uno” in the Tyrrhenian Sea are reported. Volatile Organic Compounds (VOCs), Oxygenated Volatile Organic Compounds (OVOCs), and pollutants such as nitrogen oxides, ozone, and sulphur dioxide were monitored throughout the cruise. The shallow waters at ten sites of the investigated area were also analyzed. Organic compounds such as n-alkanes showed a bimodal distribution with a maximum at C5–C6 and C10–C11 at sites the most affected by anthropic impact, whereas remote sites showed a unimodal distribution with maximum at C10–C11. The most abundant atmospheric OVOC was acetone (3.66 μg/m3), accounting for 38%; formaldehyde (1.23 μg/m3) and acetaldehyde (0.99 μg/m3) made up about 22–29% of the total. The influence of some natural sources as volcanoes, in the southern part of the Tyrrhenian Sea near the Aeolian arc was studied. This source did not induce any noticeable effect on the total amount of hydrocarbons nor on the levels of trace gases such as CFCs, whereas the trends of sulphur dioxide seemed to confirm a possible contribution. The impact of underwater emissions was observed near the Panarea and Vulcano islands, where lower pHs, high levels of Fe and Mn, and diagnostic of vent activity, were measured.