High soil pH has been highlighted as a constraint to the restoration of heathland on ex-arable land. Previous studies at the Minsmere Reserve of the Royal Society for the Protection of Birds (RSPB) in England have shown that it is possible to acidify ex-arable soils using elemental sulfur and bracken litter, although sulfur (S) is more effective. Current recommendations suggest that 4 tS/ha need to be applied to reduce soil pH below pH 4, control vigorous ruderal species, and create conditions suitable for Calluna vulgaris (heather) establishment. However, S is relatively expensive, and as bracken litter is moderately abundant within the reserve, it made economic sense to evaluate the potential for mixing S with bracken to see if adequate pH reductions could be achieved at lower S rates. Accordingly an experiment was designed to test the effects of combining S (0–8 t S/ha) and bracken litter (0–10 cm depth layers) on (1) soil pH, (2) cover of ruderal species, and (3) the developing plant community. Significant interactions were detected, especially in the period immediately after application. Where bracken litter was applied the soil pH fell immediately; in contrast, S took at least six months to start reducing pH. Where mixtures were applied there was a synergistic effect, which produced a lower pH than the S or bracken litter applied alone. These effects were most marked at low S application rates, between 0.5–4 t S/ha. The effects of the bracken litter addition also reduced the growth of ruderal species in the period immediately after application, probably through a combination of acidification and physical smothering. There is, therefore, a clear potential to acidify ex-arable soils using combinations of S and bracken litter in schemes designed to restore Calluna heathland.