Apart from influencing the amount of leaf-deposited particles, tree crown morphology will influence the local distribution of atmospheric particles. Nevertheless, tree crowns are often represented very rudimentary in three-dimensional air quality models. Therefore, the influence of tree crown representation on the local ambient PM10 concentration and resulting leaf-deposited PM10 mass was evaluated, using the three-dimensional computational fluid dynamics (CFD) model ENVI-met® and ground-based LiDAR imaging. The modelled leaf-deposited PM10 mass was compared to gravimetric results within three different particle size fractions (0.2–3, 3–10 and >10 μm), obtained at 20 locations within the tree crown. Modelling of the LiDAR-derived tree crown resulted in altered atmospheric PM10 concentrations in the vicinity of the tree crown. Although this model study was limited to a single tree and model configuration, our results demonstrate that improving tree crown characteristics (shape, dimensions and LAD) affects the resulting local PM10 distribution in ENVI-met. An accurate tree crown representation seems, therefore, of great importance when aiming at modelling the local PM distribution.