Dendrimers are structurally precise molecules, whose peripheral layer provides ample sites for anchoring functional groups of different charges and charge densities. This characteristic renders them capability of providing numerous target functional groups on the surface of filtration membranes when modified by dendrimers. Consequently, there has been a growing interest in dendrimer-modified membranes. In this study, we investigated the engineering of polyvinylidene fluoride (PVDF) membranes using polyamidoamine (PAMAM) dendrimers anchoring different functional groups to tune the charges and charge density of membranes to enable microporous membranes for separation of charged macromolecules. PVDF membranes were functionalized by grafting PAMAM-G3.0 (generation 3) dendrimers with amine groups onto their surfaces and internal surfaces of membrane pores. Subsequently, the peripheral functional groups of dendrimers on the membranes were replaced by carboxyl groups, quaternary ammonium groups, or sulfonic acid groups for charges of different nature and densities. Surface chemical properties, electrical properties, and morphology were characterized using various techniques, including attenuated total reflectance Fourier-transform infrared (ATR-FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and surface zeta potential measurement. The filtration performance of both PVDF and modified membranes was evaluated using polyethylene oxide (PEO), polyacrylic acid (PAA), and whey protein filtration. Among the modified membranes, the G3PA membranes, with carboxyl functional groups, exhibited the most effective whey protein separation performance. The whey protein rejection and permeate flux of the G3PA membranes were 79 % and 30.3 LMH, respectively. As a comparison, the whey protein rejection and permeate flux of the pristine PVDF membranes were 58.9 % and 15.3 LMH, respectively.