Conducting　polymers　(CPs),　including　poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)　(PEDOT:PSS),　are　promising　coating　materials　for　neural　electrodes.　However,　the　weak　adhesion　of　CP　coatings　to　substrates　such　as　platinum–iridium　is　a　significant　challenge　that　limits　their　practical　application.　To　address　this　issue,　we　used　femtosecond　laser-prepared　hierarchical　structures　on　platinum–iridium　(Pt–Ir)　substrates　to　enhance　the　adhesion　of　PEDOT:PSS　coatings.　Next,　we　used　cyclic　voltammetry　(CV)　stress　and　accelerated　aging　tests　to　evaluate　the　stability　of　both　drop　cast　and　electrodeposited　PEDOT:PSS　coatings　on　Pt–Ir　substrates,　both　with　and　without　hierarchical　structures.　Our　results　showed　that　after　2000 CV　cycles　or　five　weeks　of　aging　at　60 °C,　the　morphology　and　electrochemical　properties　of　the　coatings　on　the　Pt–Ir　substrates　with　hierarchical　structures　remained　relatively　stable.　In　contrast,　we　found　that　smooth　Pt–Ir　substrate　surfaces　caused　delamination　of　the　PEDOT:PSS　coating　and　exhibited　both　decreased　charge　storage　capacity　and　increased　impedance.　Overall,　enhancing　the　stability　of　PEDOT:PSS　coatings　used　on　common　platinum–iridium　neural　electrodes　offers　great　potential　for　improving　their　electrochemical　performance　and　developing　new　functionalities.　Graphic　abstract:　(Figure　presented.).　©　Zhejiang　University　Press　2024.