Dispersive Raman spectroscopy with excitation by a red diode laser is suitable for quantitative crystallinity measurements in powders for pulmonary drug delivery. In spray-dried mixtures of salmon calcitonin and mannitol, all three crystalline polymorphs of mannitol and amorphous mannitol were unambiguously identified and their mass fractions were measured with a limit of quantification of about 5%. The instrument design offered high sensitivity and adequate background suppression, resulting in a low limit of detection in the range of 0.01% to 1%. This spectroscopy method has significant advantages over established techniques regarding specificity, sensitivity, and sample requirements.