Titanium that is covered with a native oxide layer is widely used as an implant material; however, it is only passively incorporated in the human bone. To increase the implant-bone interaction, one can graft multifunctional phosphonic compounds onto the implant material. Phosphonate groups show excellent adhesion properties onto metal oxide surfaces such as titanium dioxide, and therefore, they can be used as anchor groups. Here, we present an alternative coating material composed of phosphonate surface-functionalized polystyrene nanoparticles synthesized via free radical copolymerization in a direct (oil-in-water) miniemulsion process. Two types of functional monomers, namely, vinylphosphonic acid (VPA) and vinylbenzyl phosphonic acid (VBPA), were employed in the copolymerization reaction. Using VBPA as a comonomer leads to particles with a higher density of surface phosphonate groups in comparison to those obtained with VPA. VBPA-functionalized particles were used for the coating formation on the titanium surface. The particles monolayer was investigated by scanning electron microscopy (SEM) and atomic force microscopy (AFM) employing titanium and silicium tip with the native OH groups. Force versus distance curves proves the strong adhesion between the phosphonated particles and the titanium (or silicium) surfaces in contrast to the nonfunctionalized polystyrene particles. Finally, as a proof of concept, the particles adhered to the surface were further used to nucleate hydroxyapatite, which has high potential for bioimplants.