Developing　rational　regeneration　protocol　to　upgrade　spent　cathode　material　for　their　usage　in　next　generation　lithium-ion　batteries　(LIBs)　can　alleviate　resource　stress　and　benefit　environment　and　carbon　neutrality.　This　work　demonstrates　that　direct　regeneration　of　spent　LiCoO2(LCO)　encounters　the　negative　effects　of　Al　impurity,　which　is　a　common　impurity　in　the　spent　LIB　materials　introduced　during　battery　cycling　and　disassembly　process.　Our　microanalysis　show　that　Al　impurity　tends　to　segregate　on　the　LCO　surface　during　the　direct　regeneration　process,　which　not　only　causes　poor　surface　regeneration　but　also　degenerates　the　surface　modification　effect　for　upgrading　purpose.　We　therefore　propose　a　one-pot　protocol　by　using　a　bifunctional　solution　to　realize　Al　impurity　removal　and　Ti　surface　coating　simultaneously,　which　successfully　upgrade　the　spent　LCO　for　high　voltage　and　high-power　usage.　The　upgraded　LCO　cathode　can　achieve　90　%　and　97　%　capacity　retentions　at　0.2C　and　2C　rates　after　2.8-4.5　V　100　cycles,　and　their　initial　specific　capacity　is　180　mAh/g　and　149　mAh/g,　respectively.　The　microstructure　characterizations　in　this　work　provide　in-depth　understanding　of　the　direct　regeneration　process,　which　is　essential　for　understanding　and　optimizing　the　recycling　process.　Further　economic　analysis　show　that　the　established　regeneration　protocol　holds　promise　for　realizing　large-scale　industrial　recycling　process　of　spent　LCO.