The removal of soluble organic matter in water, especially that of dissolved dyes, is an important research topic in the field of sewage treatment. In this article, mussel biometic chemical deposition was performed by catechol and polyethyleneimine (PEI) in polyvinydene fluoride (PVDF) solution to increase the surface hydrophilicity and regulate pore structure of PVDF hybrid membranes with hydrophilic units, and the performance of filtration dye aqueous solution was evaluated. The occurrence of chemical deposition was confirmed by new peaks in both IR and XPS spectra. The water contact angle of membrane surface is decreased from 84° to 43°. The pH value of isoelectric point of the membrane surface increases from 3.54 to 4.26. SEM images show that there emerge more tiny channels just below the cortex of membrane. The filtration test of 10 mg/L crystal violet (CV) and methyl blue solution provides 99% and 97% rejection rate by M-2, which contains 1.0% hydrophilic units. The retention for CV decreases to 74.1% after 50 h filtration with stable water flux.