Pharmaceutical tablet properties, including surface roughness, gloss and temperature, are determined in real-time using Raman spectroscopy. A plurality of coated pharmaceutical tablets are provided having a distribution of known values of a surface property to be modeled. The Raman spectrum of each coated tablet is acquired to generate a distribution of Raman spectra. A correlative model is then developed based upon the distribution of the acquired Raman spectra relative to the distribution of the known values of the measured property. The Raman spectrum of a pharmaceutical tablet is then acquired during and/or after a coating process, and the value of the surface property of the tablet is determined using the correlative model. The steps associated with model development are carried out off-line, whereas the step or steps associated with acquiring the Raman spectra of the pharmaceutical tablet during (preferable) or after online coating process(es) are carried out on-line using a remote, fiber-coupled probe.