In article number 1802392, Lev T. Perelman and co-workers report a quantitative label-free surface-enhanced Raman spectroscopy (SERS) method for identifying and quantifying drugs at ultralow concentrations. Self-assembled gold nanoclusters entrap drug molecules and laser light excites the surface plasmon resonance, yielding a large SERS signal from the molecule trapped near the hot spot, allowing measurements of drugs in urine samples at clinically relevant concentrations.