treatment technology an extremely tough task. [1] Currently, membrane separation technology has become the main channel to remediate the water environment attribu ting to its advantages, such as environ mental sustainability and energy saving. [2] Particularly, graphene oxide (GO) and carbon nanotubes (CNTs), have attracted comprehensive attention on constructing multifunctional separation membranes in the scientific field. [3] For one thing, they possess high surface areas that are ben eficial to achieve effective adsorption with watersoluble pollutants (dye molecules, bacteria, et al.). [4] For another, they can be taken as secondary reaction platforms for designing functional membranes through chemical crosslinking, interface assembly, and nanoparticle modification, which will enhance their capture ability for target compounds. [5] To date, the research on carbonbased membranes with versatility has brought inspiring achievements. For example, Liu and coworkers have designed a SiO 2 /GO composite mem brane through the modification of SiO 2 nanoparticle and eth ylenediamine. [6] It can purify the oilinwater (O/W) emulsion with the flux of 470 L m −2 h −1 and high retention capacity for dye molecules. Chen et al. have constructed a series of super hydrophilic CNTsbased composite membranes via hydrophilic Membrane separation is recognized as one of the most effective strategies to treat the complicated wastewater system for economic development. However, serious membrane fouling has restricted its further application. Inspired by sphagnum, a 0D/2D heterojunction composite membrane is engineered by depositing graphitic carbon nitride nano/microspheres (CNMS) with plentiful wrinkles onto the polyacrylic acid functionalized carbon nanotubes (CNTs-PAA) membrane through hydrogen bond force. Through coupling unique structure and chemistry properties, the CNTs-PAA/CNMS heterojunction membrane presents superhydrophilicity and underwater superoleophobicity. Furthermore, thanks to the J-type aggregates during the solvothermal process, it is provided with a smaller bandgap (1.77 eV) than the traditional graphitic carbon nitride (g-C 3 N 4) sheets-based membranes (2.4-2.8 eV). This feature endows the CNTs-PAA/CNMS membrane with superior visible-lightdriven self-cleaning ability, which can maintain its excellent emulsion separation (with a maximum flux of 5557 ± 331 L m −2 h −1 bar −1 and an efficiency of 98.5 ± 0.6%), photocatalytic degradation (with an efficiency of 99.7 ± 0.2%), and antibacterial (with an efficiency of ≈100%) ability even after cyclic experimental processes. The excellent self-cleaning performance of this all-in-one membrane represents its potential value for water purification.