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Volcanic ash contributed significantly to particulate matter (PM) in Iceland following the eruptions in Eyjafjallajökull 2010 and Grímsvötn 2011. This study aimed to investigate the association between different PM sources and emergency hospital visits for cardiorespiratory causes from 2007 to 2012. Indicators of PM₁₀ sources; “volcanic ash”, “dust storms”, or “other sources” (traffic, fireworks, and re-suspension) on days when PM₁₀ exceeded the daily air quality guideline value of 50 µg/m³ were entered into generalized additive models, adjusted for weather, time trend and co-pollutants. The average number of daily emergency hospital visits was 10.5. PM₁₀ exceeded the air quality guideline value 115 out of 2191 days; 20 days due to volcanic ash, 14 due to dust storms (two days had both dust storm and ash contribution) and 83 due to other sources. High PM₁₀ levels from volcanic ash tended to be significantly associated with the emergency hospital visits; estimates ranged from 4.8% (95% Confidence Interval (CI): 0.6, 9.2%) per day of exposure in unadjusted models to 7.3% (95% CI: −0.4, 15.5%) in adjusted models. Dust storms were not consistently associated with daily emergency hospital visits and other sources tended to show a negative association. We found some evidence indicating that volcanic ash particles were more harmful than particles from other sources, but the results were inconclusive and should be interpreted with caution.