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The crystal structure of the heterocyclic compound 2‐(4‐methoxyphenyl)‐7‐phenylpyrazolo[1,5‐c]pyrimidine, C19H15N3O, has been determined and its self‐assembly on the surface of graphite has been examined using atomic force microscopy (AFM). The title compound crystallized in the monoclinic space group P21/c, with two independent molecules in the asymmetric unit. The packing of the L‐shaped molecules in the crystal is governed by arene interactions, in the absence of any conventional hydrogen‐bonding interactions. The packing arrangement reveals four types of dimeric motifs stabilized by π–π and C—H...π interactions. At low coverage, molecules assemble into long needle‐like islands on the graphite surface. High‐resolution AFM images reveal that the molecules interact through weak noncovalent interactions between the aromatic H atoms and the methoxy O atoms. [ABSTRACT FROM AUTHOR]