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Evidence for oscillation in monolithic molecular single crystals of a  thiophene/phenylene co‐oligomer is reported. The laser oscillations (see Figure) are characterized by naturally formed crystal facet cavities with molecular‐scale flatness. The multimode laser oscillation in a Fabry–Pérot resonator is characterized by sharply resolved spectroscopic lines with their full width at half maximum down to only 38 pm. The laser oscillation is characterized by the presence of a well‐defined threshold.