Adjustable　lubrication　aims　to　achieve　active　control　of　the　relative　motion　of　the　friction　interface,　providing　a　new　idea　for　intelligent　operation.　A　new　phenomenon　of　sudden　changes　of　friction　coefficient　(COF)　in　the　poly(vinylphosphoric　acid)　(PVPA)　superlubricity　system　by　mixing　different　lubricants,　was　found　in　this　study.　It　was　found　that　anions　were　the　critical　factor　for　the　COF　change.　The　change　degrees　of　the　COF　were　investigated　by　a　universal　micro　tribometer　(UMT).　A　quartz　crystal　microbalance　(QCM)-D　was　used　to　analyze　the　adsorption　quantity　of　anions　on　the　PVPA　surface.　The　hydratability　of　the　PVPA　interface　was　controlled　by　changing　the　anionic　properties　(the　amount　of　charge　and　structure),　thus　regulating　the　COF.　The　adsorption　difference　of　anions　is　an　important　reasoning　of　how　anionic　properties　can　regulate　the　hydratability.　It　was　analyzed　by　molecular　dynamics　simulation.　For　anions　carrying　different　numbers　of　charges　or　double　bonds,　the　adsorption　quantity　of　anions　was　mainly　affected　by　the　adsorption　degree　on　the　PVPA　surface,　while　the　adsorption　quantity　of　anions　with　different　molecular　configuration　was　synergistically　regulated　by　the　adsorption　degree　and　adsorption　area　of　anions　on　the　PVPA　surface.　This　work　can　be　used　to　develop　smart　surfaces　for　applications.