Design　and　fabrication　of　feasible　remediation　composites　for　total　Cr　(Cr(T))　removal　is　still　challenging　but　urgently　required.　Herein,　eco-friendly　expanded　vermiculite　(VE)　is　integrated　with　a　photoactive　covalent　organic　framework　(COF)　polymer,　in　which　photoinduced　electrons　of　surface　anchored　COF　can　freely　transfer　to　Cr(VI)　for　chemical　reduction,　and　layered　expanded　VE　allows　ion　exchange　between　resultant　Cr(III)　cations　and　interlayered　K+,　Ca2+,　Mg2+,　Na+,　etc.　The　Cr(T)　removal　capacities　of　the　surface-modified　VE　with　important　parameters　(solution　pH　value,　initial　Cr(VI)　concentration,　etc.)　are　discussed　extensively　to　understand　how　to　select　the　best　conditions　for　optimum　Cr(T)　removal　performance.　More　interestingly,　from　a　circular　economy　view　point,　spent　Cr-loading　VE-based　waste　can　serve　as　a　photocatalyst　towards　oxidation　conversion　of　ciprofloxacin　and　NO　gas　subsequently.　Explanations　for　different　effects　on　physicochemical　properties　as　well　as　catalytic　activities　of　the　reused　Cr-loading　waste　are　given.　This　strategy　could　provide　valuable　and　promising　contribution　towards　the　development　of　sustainable　low-cost　mineral　materials　for　Cr　(T)　removal.　These　findings　also　shed　new　light　on　the　research　of　recycling　spent　photocatalyst　for　resource　and　reutilization.