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A novel polyvinylidene fluoride (PVDF) tree-like nanofiber membrane (PVDF-TLNM) was fabricated by adding tetrabutylammonium chloride (TBAC) into a PVDF spinning solution via one-step electrospinning. The structure of the prepared membranes was characterized by field emission scanning electron microscopy (FE-SEM), Fourier transform infrared spectroscopy (FT-IR) and pore size analysis, and the hydrophilic property and microfiltration performance were also evaluated. The results showed that the tree-like nanofiber was composed of trunk fibers and branch fibers with diameters of 100–500 nm and 5–100 nm, respectively. The pore size of PVDF-TLNM (0.36 μm) was smaller than that of a common nanofiber membrane (3.52 μm), and the hydrophilic properties of the membranes were improved significantly. The PVDF-TLNM with a thickness of 30 ± 2 μm showed a satisfactory retention ratio of 99.9% against 0.3 μm polystyrene (PS) particles and a high pure water flux of 2.88 × 104 L·m−2·h−1 under the pressure of 25 psi. This study highlights the potential benefits of this novel PVDF tree-like nanofiber membrane in the membrane field, which can achieve high flux rates at low pressure.