Tight ultrafiltration (TUF) membranes featuring specific pore sizes are increasingly developed to bridge the gap between nanofiltration and ultrafiltration. So far, a wealth of efforts has been devoted to tackle the limitation found in TUF, but there still lacks a facile accessibility to upgrade TUF membranes with simultaneously improved permeance and selectivity. Herein, we report a large-pore covalent organic framework (LP-COF) as the building material to prepare ultra-permeable TUF membranes for fast separations. The LP-COF layers with an exceptionally large aperture size of up to ~3.6 nm are synthesized on macroporous substrates through a unidirectional diffusion method. The resultant LP-COF layers show a moderate crystallinity and low thickness down to ~60 nm, and allow ultrafast water permeation. Surprisingly, the optimal LP-COF membrane exhibits an unprecedented water permeance of ~3147 L m−2 h−1 MPa−1 with a high Congo red rejection (~92.6%), which is basically unchanged after several cycles of filtration. Moreover, the large-pore channels enable an unimpeded pass of ions, thus affording the membrane an excellent dye/salt separation competence, and largely exceeding state-of-the-art membranes. Therefore, this work opens up a new opportunity in producing high-performance TUF membranes by large-pore COFs for rapid and precise separations.