In　this　paper,　a　3D　hierarchical　layered　double　hydroxide　(LDH)/carbon　sphere　(CS)　composite　was　prepared　via　self-assembly　method.　After　calcination,　the　hollow　structure　with　high　surface　area　was　formed　due　to　removing　the　carbon　core,　meanwhile,　LDH　turned　into　layered　double　oxide　(LDO)　which　exhibited　superior　anion　adsorption　capacity.　The　formation　of　the　prepared　material　was　confirmed　and　characterized,　and　the　adsorption　mechanism　of　the　obtained　material　for　different　charge　anionic　dyes　was　further　discussed　in　detail.　Under　the　optimal　conditions,　the　maximum　adsorption　capacities　of　the　prepared　materials　for　amaranth　and　Orange　II　were　638.634　and　849.674　mg/g,　separately,　which　revealed　that　the　materials　can　be　applied　into　the　effective　adsorption　of　anionic　dyes,　especially　those　with　less　charges.