In a recent paper (New J. Chem., 2001, 25, 1520), we have analysed crystal structures of some N-aryl pyrimidinones. Based on the occurrence of two-dimensional layers in six out of nine crystals, we proposed that self-assembly in these structures might be analysed in terms of the stacking of 2D hydrogen-bonded layers. We show herein that meta-substituted phenyl pyrimidinones (Br, I, F, NO2, Me, OMe) have an overwhelming preference for the 2D polar ...