between the atmosphere and the hydrosphere and by spanning about 70% of the Earth's surface, the sea-surface microlayer (sea-SML) is regarded as a fundamental component in air–sea exchange processes and in biogeochemical cycling. Although having a minor thickness of <1000 µm, the elusive SML is long known for its distinct physicochemical characteristics compared to the underlying water, e.g., by featuring the accumulation of dissolved and particulate organic matter, transparent exopolymer particles (TEP), and surface-active molecules. Therefore, the SML is a gelatinous biofilm, maintaining physical stability through surface tension forces. It also forms a vast habitat for different organisms, collectively termed as neuston with a recent global estimate of 2 × 1023 microbial cells for the sea-SML. Life at air–water interfaces has never been considered easy, mainly because of the harsh environmental conditions that influence the SML. However, high abundances of microorganisms, especially of bacteria and picophytoplankton, accumulating in the SML compared to the underlying water were frequently reported, accompanied by a predominant heterotrophic activity. This is because primary production at the immediate air–water interface is often hindered by photoinhibition. However, some exceptions of photosynthetic organisms, e.g., Trichodesmium, Synechococcus, or Sargassum, show more tolerance towards high light intensities and, hence, can become enriched in the SML. Previous research has provided evidence that neustonic organisms can cope with wind and wave energy, solar and ultraviolet (UV) radiation, fluctuations in temperature and salinity, and a higher potential predation risk by the zooneuston. Furthermore, wind action promoting sea spray formation and bubbles rising from deeper water and bursting at the surface release SML-associated microbes into the atmosphere. In addition to being more concentrated compared to planktonic counterparts, the bacterioneuston, algae, and protists display distinctive community compositions compared to the underlying water, in both marine and freshwater habitats. Furthermore, the bacterial community composition was often dependent on the SML sampling device being used. While being well defined with respect to bacterial community composition, little is known about viruses in the SML, i.e., the virioneuston. This review has its focus on virus–bacterium dynamics at air–water interfaces, even if viruses likely interact with other SML microbes, including archaea and the phytoneuston, as can be deduced from viral interference with their planktonic counterparts. Although viruses were briefly mentioned as pivotal SML components in a recent review on this unique habitat, a synopsis of the emerging knowledge and the major research gaps regarding bacteriophages at air–water interfaces is still