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Electrophoretic deposition (EPD) of platinum nanoparticles (PtNPs) on platinum–iridium (Pt–Ir) neural electrode surfaces is a promising strategy to tune the impedance of electrodes implanted for deep brain stimulation in various neurological disorders such as advanced Parkinson’s disease and dystonia. However, previous results are contradicting as impedance reduction was observed on flat samples while in three-dimensional (3D) structures, an increase in impedance was observed. Hence, defined correlations between coating properties and impedance are to date not fully understood. In this work, the influence of direct current (DC) and pulsed-DC electric fields on NP deposition is systematically compared and clear correlations between surface coating homogeneity and in vitro impedance are established. The ligand-free NPs were synthesized via pulsed laser processing in liquid, yielding monomodal particle …