Cross-linked fluoroalkyl end-capped co-oligomeric nanoparticle-encapsulated fullerenes, prepared by deprotecting a fluoroalkyl end-capped isocyanatoethyl methacrylate 2-butanone oxime adduct-1-hydroxy-5-adamantylacrylate co-oligomer in the presence of fullerene, were of well-defined size in the nanometer range (28-82 nm) and exhibited good dispersibility in a variety of solvents such as methanol, ethanol, isopropyl alcohol, tetrahydrofuran, N,N-dimethylformamide, dimethyl sulfoxide, and 1,2-dichloroethane. Transmission electron microscopy images also showed that these nanocomposites were particles with a mean diameter of 45 nm and that the fullerenes were tightly encapsulated into fluorinated nanoparticle cores. In methanol, these fluorinated nanoparticles emitted fluorescence related to the presence of fullerene and were applied in the Surface modification of traditional organic polymers Such as poly(methyl methacrylate) (PMMA) to effect good oleophobicity imparted by fluorine on the modified film surfaces. Interestingly. a higher fluorescent intensity of fullerene was observed on the modified PMMA surfaces, although the reverse side of these film surfaces yielded an extremely weal, fluorescent intensity. More interestingly, a fluorescence microscopy image of the cross-section of the modified PMMA film showed that encapsulated fullerene was arranged regularly above the modified PMMA film surface.