Ashfall from volcanic eruptions endangers crop production and food security while jeopardising agricultural livelihoods. As populations in the vicinity of volcanoes continue to grow, strategies to reduce volcanic risks to and impacts on crops are increasingly needed. Current models of crop vulnerability to ash are limited. They also rely solely on ash thickness (or loading) as the hazard intensity metric and fail to reproduce the complex interplay of other volcanic and non-volcanic factors that drive impact. Amongst these, ash retention on crop leaves affects photosynthesis and is ultimately responsible for widespread damage to crops. In this context, we carried out greenhouse experiments to assess how ash grain size, leaf pubescence, and humidity conditions at leaf surfaces influence the retention of ash (defined as the percentage of foliar cover coated with ash) in tomato and chilli pepper plants, two crop types commonly grown in volcanic regions. For a fixed ash mass load (∼570 g m−2), we found that ash retention decreases exponentially with increasing grain size and is enhanced when leaves are pubescent (such as in tomato plants) or when their surfaces are wet. Assuming that leaf area index (LAI) diminishes with ash retention in tomato and chilli pepper plants, we derived a new expression for predicting potential crop yield loss after an ashfall event. We suggest that the measurement of crop LAI in ash-affected areas may serve as an impact metric. Our study demonstrates that quantitative insights into crop vulnerability can be gained rapidly from controlled experiments. We advocate this approach to broaden our understanding of ash–plant interactions and to validate the use of remote sensing methods for assessing crop damage and recovery at various spatial and time scales after an eruption.