A poly(N-acryloyl glycinamide) (PNAGA) conducted smart graphene oxide (GO) membrane was fabricated, which exhibits a unique “thermo-schizophrenic” phenomenon. The combination of supramolecular interactions at different temperatures and confined nano-channels was considered to arouse such new properties. The aggregation of PNAGA fragments, homogeneously polymer distribution, and chain stretching based on supramolecular interactions at different temperatures, cause the “thermo-schizophrenic” feature. The limited size of the nano-channel constructed by GO also contributed to this newfangled adjustable superfluid phenomenon. Overall, this work provides a substantial and definitive complementarity to the unique application of PNAGA at different temperatures. It induces a way to prove the significance and specialty of the confined spacing in designing the 2D-nanofiltration membrane. This strategy also gives valuable guidance for designing smarter materials using a single homopolymer.