Herein, we reported an efficient and green approach to synthesize a novel 2D BiOBr/ZnAl1.8Fe0.2O4 hetero-junction photocatalysts by using tissue paper as template. The as-prepared sample was composed of microfibers interspersed with each other to form 2D structure, and each microfiber was assembled by BiOBr microspheres and ZnAl1.8Fe0.2O4 nanoparticles derived from layered double hydroxides precursors. The obtained samples exhibited both high adsorption capacity and superior photocatalytic activity in removal of antibiotics and anionic dyes from water. The maximum adsorption capacities of BiOBr/ZnAl1.8Fe0.2O4 towards Congo Red (CR) and Doxycycline (DC) were 210.5 and 227.4 mg g(-1), respectively, and the pseudo-second order kinetic model describes the adsorption process well. The as-synthesized samples also exhibited superior photocatalytic activity toward low concentration of CR and DC under simulated sunlight irradiation thanks to its high charge separation ratio, hierarchically porous morphology and synergic adsorption-photocatalysis effect.