Porous organic frameworks (POFs) based membranes have potential applications in molecular filtration, despite the lack of a corresponding study. This study reports an interesting strategy to get processable POFs dispersion and a novel ultrathin sandwich-like membrane design. It was accidentally found that the hydrophobic N-rich Schiff based POFs agglomerates could react with lithium-ethylamine and formed stable dispersion in water. By successively filtrating the obtained POFs dispersion and graphene oxide (GO), we successfully prepared ultrathin sandwich-like hybrid membranes with layered structure, which showed significantly improved separation efficiency in molecular filtration of organic dyes. This study may provide a universal way to the preparation of processable POFs and their hybrid membranes with GO.