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The efficacy of electrodes that are chronically implanted and used in the context of deep brain stimulation (DBS) for the treatment of neurological disorders critically depends on stable impedance. Platinum–iridium electrodes were coated with laser-generated platinum nanoparticle colloids (PtNPs) via electrophoretic deposition using pulsed direct currents (DC-EPD). Uncoated electrodes were used as controls. In vitro, electrodes were stimulated for four weeks in a 0.9% NaCl solution. For the in vivo (rats) study, coated electrodes were implanted in the left and uncoated control electrodes in the right subthalamic nucleus (STN). After two weeks of recovery, electrodes were stimulated for four weeks. Impedance measurements were conducted after each week of stimulation, both in vivo and in vitro. NP-coating resulted in a significant and long-lasting reduction in electrode impedance (p < 0.05) over four weeks of in vitro stimulation. Despite an initial increase in impedance after intracranial implantation, the impedance of the NP-coated electrodes was also reduced during in vivo stimulation over four weeks. NP-coated electrodes had a lower fluctuation of impedance during stimulation compared to uncoated electrodes both in vitro and in vivo (p < 0.05). Laser-generated PtNPs applied to electrodes by pulsed DC-EPD lead to lower and more stable electrode impedance during chronic stimulation, with the potential to enhance the performance of DBS systems during chronic use. [ABSTRACT FROM AUTHOR]