Malachite green isothiocyanate (MGITC) is frequently used as a surface bound Raman reporter for metal nanoparticle-enabled surface enhanced Raman scattering (SERS). To date, however, no study has focused on the application of MGITC for the formation of stable "hot-spot" aggregates for Raman imaging applications. Herein we report a method to produce a series of suspensions of MGITC functionalized gold nanoparticles (MGITC-AuNPs) that at one extreme consist primarily of monomers and at the other extreme as mixtures of multimers and monomers. Monomer and multimer morphologies were characterized by scanning electron microscopy and atomic force microscopy using a reliable spin-coating deposition sampling method. The multimers generally include 2, 3, or 4 individual AuNPs with an average number of 3 ± 1. The number of multimers produced in a given suspension was found to be dependent on the volume and concentration of MGITC initially applied. The surface binding of MGITC to both monomeric and multimeric MGITC-AuNPs was investigated by Raman and SERS, and the degree of aggregation in the multimer suspension was evaluated based upon the measured variation of the MGITC SERS intensity of the AuNPs. Using an estimated extinction coefficient of 1.22 ± 0.41 × 10(11) M(-1) cm(-1) at ≈850 nm for the localized surface plasmon resonance (LSPR) band of the MGITC-AuNP multimers, the multimer concentrations were calculated by Beer's Law.