Herein, a NiAl-LDH/COF composite was fabricated by directly synthesizing an imine-based COF on the NiAl-LDH surface and its identification was followed by fourier-transform infrared spectroscopy, X-ray diffraction, field-emission scanning electron microscopy, Energy dispersive X-ray spectrometry, Brunauer-Emmett-Teller, and simultaneous thermal analysis. This composite was utilized as a catalyst with a high surface area for the Knoevenagel condensation. Under low loading amount (10 mg), extremely short reaction times (5–25 min) and 25 °C, NiAl-LDH/COF composite promotes the condensation of malononitrile with various aldehydes to produce benzylidenemalononitrile derivatives with high yields (82–96 %) and good recyclability. The NiAl-LDH/COF was reused four times without a noteworthy loss in catalytic performance.