Polymer　coatings　can　effectively　improve　the　surface　tribological　properties　of　human　implant　materials,　thereby　increasing　their　service　life.　In　this　study,　poly(vinylsulfonic　acid,　sodium　salt)　(PVS),　poly(acrylic　acid)　(PAA)　and　poly(vinylphosphonic　acid)　(PVPA)　were　used　to　modify　Ti6Al4V　surfaces.　Experimental　analyses　were　combined　with　molecular　simulation　to　explore　the　regulation　mechanism　of　special　functional　groups　contained　in　polymer　molecular　chains　on　the　tribological　properties　of　modified　surfaces.　In　addition,　the　bearing　capacities　and　velocity　dependence　of　different　polymer　modified　surfaces　during　friction　were　also　explored.　The　PVS　coating,　due　to　physical　adsorption,　can　have　an　anti-friction　effect　under　NaCl　solution　lubrication,　but　is　not　durable　under　long-term　or　repeated　usage.　Both　PAA　and　PVPA　molecular　chains　can　form　chemical　bonds　with　Ti6Al4V.　Phosphate　acid　groups　can　firmly　bind　to　the　substrate,　and　the　adsorption　of　salt　ions　and　water　molecules　can　form　a　hydrated　layer　on　the　PVPA　coating　surface,　achieving　ultra-low　friction　and　wear.　The　adsorption　of　salt　ions　would　aggravate　the　surface　wear　of　the　PAA-modified　Ti6Al4V　due　to　the　unfirm　binding　of　carboxyl　groups　to　the　substrate,　resulting　in　a　high　friction　coefficient.　This　study　can　provide　effective　guidance　for　the　design　of　modified　polymer　coatings　on　metals.　©　2023　by　the　authors.