Since EC and macrophages are key players in the onset and progression of chronic vascular inflammation, the focus of this paper was to synthesize, characterize, and further investigate the anti-inflammatory potential of novel PCA-functionalized dextran-coated magnetic nanoparticles (MNP-Dex/PCA) on these cells by examining the protein expression of various pro-inflammatory molecules (e.g., IL-1β, TNF-α, IL-6, MCP-1, and CCR2) and signaling molecules involved in inflammation (e.g., NF-kB, p38-α, and ERK 1/2). This evidence concerns the gene TNF and inflammatory response.