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Engineered self-assembled monolayer (SAM) substrates were successfully illustrated as a high throughput polymorph screening method for cocrystals. In this study, we have obtained new polymorphs of the cocrystals of caffeine and oxalic acid (2 : 1 molar ratio). This is evidenced by the Raman spectra, which showed new peaks at 1076, 1588 and 1602 cm−1. In addition, the XRD diffraction pattern exhibited a new peak at 30.0°, further confirming the presence of new polymorphs.