Using an inductively coupled plasma, hydrogenated amorphous silicon (a-Si:H) films have been prepared at very low temperatures (<50 °C) to provide crystalline silicon (c-Si) surface passivation. Despite the limited nanostructural quality of the a-Si:H bulk, a surprisingly high minority carrier lifetime of ∼4 ms is demonstrated after a rapid thermal annealing treatment. Besides the excellent level of surface passivation, the main advantage of the low-temperature approach is the facile suppression of undesired epitaxial growth. The correlation between the a-Si:H nanostructure and the activation of a-Si:H/c-Si interface passivation, upon annealing, has been studied in detail. This yields a structural model that qualitatively describes the different processes that take place in the a-Si:H films during annealing. The presented experimental findings and insights can prove to be useful in the further development of very thin a-Si:H passivation layers for use in silicon heterojunction solar cells.