BACKGROUND: Due to cellulose of paper is abundant, inexpensive and renewable in nature, the development of paper-based materials from cellulose to substitute materials prepared by complicated chemical routes is a fascinating challenge. This work investigates a novel method for fabricating paper-based Ni-Al layered double hydroxides (LDHs)/Al2O3 composite using celluloses as template; the fabricated composite was applied to adsorb bovine serum albumin (BSA) from water. RESULTS: Scanning electron microscopy (SEM) images demonstrate the hierarchical morphologies and multiscale structures of composites at scales ranging from micro- to nano-scales. The unique macroporous structures can be directly observed by morphology analysis, and show that these materials which have potential applications in bulky biomolecules adsorption. Compared with bare LDH particles, LDHs/Al2O3 composites show a high binding capacity for BSA, where the appropriate adsorption capacity is achieved at neutral pH. The equilibrium data for BSA adsorption onto composites are found to be well described by the Langmuir isotherm model, while the kinetic data are well-fitted to the pseudo-second-order model. CONCLUSION: Since the BSA adsorbed composites show near complete (over 95%) desorption in a high negative charge density of salt solution, suggesting that the paper-based Ni-Al LDHs/Al2O3 composites are practically usable for BSA separation. (C) 2013 Society of Chemical Industry