The manipulation of carotenoid-based hierarchical superstructures affords attractive properties that facilitate application in biology and photosynthesis. Here, tubular suprastructures formed from water-soluble amide-modified resorcinarene and β-carotene were reported, whereas microsheets were formed when β-carotene was replaced with lutein. These structures were characterized using various measurements, indicating the differences of binding sites between resorcinarene and β-carotene/lutein. Subsequently, the assembly mechanism was described by calculating the formation energy of the assemblies.