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The increased severity and prevalence of insoluble deposits formed on fuel injectors in gasoline direct injection (GDI) engines precipitates negative environmental, economic and healthcare impacts. A necessary step in mitigating deposits is to unravel the molecular compositions of these complex layered materials. But very little molecular data has been acquired. Mass spectrometry shows promise but most techniques require the use of solvents, making them unsuited for analyzing insoluble deposits. Here, we apply the high mass-resolving power and in-situ analysis capabilities of 3D OrbitrapTM secondary ion mass spectrometry (3D OrbiSIMS) to characterize deposits formed on the external tip and internal needle from a GDI injector. This is the first application of the technique to study internal GDI deposits. Polycyclic aromatic hydrocarbons (PAHs) are present up to higher maximum masses in the external deposit.