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Urban areas profoundly alter the local atmosphere, hydrology and biology, usually for the worse. Increasing the vegetative cover in urbanised areas is considered an effective way of offsetting many of the undesirable outcomes of urbanisation and is often incorporated as Green Infrastructure into urban development plans. In this paper we present a first assessment of the green cover in Irish city centres (Belfast, Cork, Derry, Dublin, Galway, Limerick and Waterford) and evaluate the environmental benefits of trees for air quality using the i-Tree Canopy software. This online software is used to conduct a spatial sample of the urban landscape and estimate tree canopy cover from which potential air quality benefits are calculated. The results show significant differences between and within city centre areas in terms of vegetative (and tree) cover; Belfast and Dublin, with less than 10% vegetative cover are in marked contrast to other cities where the average is close to 30%. Based on the findings we discuss place-based policies for improving green infrastructure in Irish cities and the evidence needed to support policies.