The movement of leukocytes to the site of inflammation in response to injury or infection is orchestrated by chemokines binding and signaling through cognate receptors. The interaction between sulfated tyrosine residues on the flexible N-terminal tail of the receptor with positively charged regions of the chemokine is one of the key recognition features that facilitates binding. In this manuscript we describe the synthesis of polymers and silica nanoparticles bearing polystyrene sulfonate brushes to mimic the sulfated tyrosine residues. We show that both the polymers and nanoparticles possess high binding affinity for the chemokine monocyte chemoattractant protein-1 (MCP-1) in monomeric and dimeric form. We also demonstrate key differences in the relative affinity for the chemokine for the free polymer versus the polymer-derived nanoparticle system.