This paper presents the results of a continuing investigation of several functionalized SPION MR contrast agents and the solid state NMR studies of plasma polymerized Allyl Alcohol thin films. Several species of functionalized SPIONs were tested; the most successful SPIONs were the melamine dendron, polyimidazole, and conjugated nucleic acid SPIONs. The study of the MR responses of the melamine dendron SPIONs determined that these SPIONs undergo reversible clustering and that their pH sensitive MR responses are due to increased clustering at pH> 4. The MR responses of the polyimidazole functionalized SPIONs (both the dopamine and carboxylate linked) indicate a pH sensitive MR response well within the physiological regime (inflection point pH ~6) as well as excellent baseline relaxivities. However, perhaps due to the low polyimidazole loading onto the SPION core, these agents were very sensitive to ionic environment. CPMAS studies of pulsed plasma polymerized allyl alcohol thin films indicated that the hydrophobic films had a more ordered structure than the hydrophilic films; however, all poly-allyl alcohol thin films had a highly amorphous structure. The use of synthetic mica as a substrate for CPMAS studies of polymer thin films is also discussed.