Luminescence　materials　have　received　extensive　attention　for　anti-counterfeiting　applications　due　to　their　low-cost　fabrication　and　simple　verification　advantages.　However,　single-emitting　encryption　can　be　easily　cracked.　Therefore,　the　development　of　multi-responsive　anti-counterfeiting　strategies　is　urgent.　Here,　we　report　a　facile　and　universal　method　to　fabricate　ultraviolet　and　infrared　excitable　inorganic-organic　hybrid　materials　that　consist　of　up-conversion　nanoparticles　(UCNPs)　and　organic　afterglow　materials.　With　this　method,　UCNPs　can　be　assembled　onto　organic　afterglow　materials　driven　by　the　electrostatic　interactions　between　the　two　com-ponents.　As　a　proof-of-concept,　a　NaYF4:　Yb,　Er　UCNPs@catechol-doped　cyanuric　acid　(cd-CA)　composite　was　designed　and　served　as　a　secret　anti-counterfeiting　ink　material.　The　security　label　using　the　hybrid　material　as　an　information　carrier　shows　multiple　encryption　signals,　such　as　fluorescence,　up-conversion,　phosphorescence,　and　infrared　thermal　imaging,　increasing　security.