The administration of levodopa/carbidopa, prodrugs that cross the blood–brain barrier and are metabolized to dopamine in the central nervous system, remains the most effective treatment for Parkinson’s disease. The development of carrier systems to increase the rate of blood–brain barrier crossing has been a challenge. In particular, buckminsterfullerene C60 is promising, due to its ability to penetrate through the skin and the gastrointestinal tract. Aiming to give theoretical support to attempts in developing levodopa/carbidopa preparations for transdermal and oral administration looking for more continuous dopamine stimulation, we present a computational study of them adsorbed on C60 fullerene in the 2–8 pH range. We use classical and quantum simulations as our computational tools. Annealing calculations were performed to explore the space of their molecular configurations to obtain optimal geometries. A detailed interpretation of their harmonic vibrational frequencies are also presented, through the analysis of their Raman and infrared spectra.