Development of sorbent materials with high selectivity and sorption capacity, easy collection and recyclability is demanding for spilled oil recovery. Although many sorption materials have been proposed, a systematic study on how they can be reused and possible performance degradation during regeneration remains absent1,2. Here we report electrospun poly (acrylonitrile) (PAN) nanomembrane sponges decorated with Mg-Al layered double hydroxide nanosheets (Mg-Al LDH), which are porous structures consisting of interconnected Mg-Al LDH nanosheets3. The Mg-Al sponges show high mass sorption capacity for toluene, reached 56 g/g, corresponding to a volume sorption capacity of 99%. The sponges are thermally and mechanically strong, oil can be squeezed out by compression, and the sponges could be easily recovered by rinsing with ethanol and can be reused as before. The electrospun Mg-Al LDH sponges maintain original structure, high capacity, and selectivity after 20 sorption and reclamation cycles. Our results suggest that practical application of LDH electrospun nanomembrane sponges in the field of spilled oil recovery is feasible4