The transport of viruses in unsaturated porous media has been a subject of great interest in recent years because of the enhanced removal of these microorganisms compared with saturated conditions. We studied the transport of bacteriophages MS2 and ϕX174, used as surrogate pathogenic viruses, at various water contents and solution chemistries in terms of pH and ionic strength (IS). The objective was to explore the interaction of viruses with the solid–water interfaces (SWI) and air–water interfaces (AWI) for a range of conditions. The experimental data were fitted with a transport model to determine the adsorption (attachment and detachment rate) parameters. Our results show that the retention of viruses in the soil column increases as water saturation decreases when the chemical conditions are favorable for adsorption (pH 7 and relatively high IS). Our analysis indicates that the enhanced retention of ϕX174 viruses at lower water contents is caused by increased attachment to the SWI and that retention by the AWI is not significant. Results obtained from a first series of experiments (pH 9 and low IS) showed insignificant attachment of MS2 viruses to both the SWI and the AWI. The MS2 breakthrough data for a second series of experiments (pH 7 and high IS) did not allow us to separate out the role of the AWI. Although attachment of MS2 viruses to the AWI cannot be ruled out in our experiments, we suspect that the increased retention of this phage under unsaturated condition was also due to enhanced attachment to the SWI. Increased attachment to the SWI under unsaturated conditions is attributed to increased mass transfer of viruses to the SWI due to a reduced diffusion length at lower water contents. Our results demonstrate that if there is any attachment to the AWI, it is reversible. When unfavorable conditions occur for attachment to the SWI, the attached viruses may be detached by moving solid–water–air contact lines (SWA).