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 surface hydrophilicity, regulate pore structure of membrane, prepared PVDF hybrid membranes with hydrophilic units and evaluated the performance of filtration dye aqueous solution. Occurrence of chemical deposition was confirmed by new peaks in both IR and XPS spectra. The water contact angle of membrane surface decreased from 84° to 43°. The pH value of isoelectric point of membrane surface increases from 3.54 to 4.26. SEM images showed that there emerged more tiny channels just below the cortex of membrane. Filtration test of 10 mg/L crystal violet (CV) and methyl blue solution provided 99% and 97% rejection rate by M-2, which contained 1.0 wt% hydrophilic units. The retention for CV decreased to 74.1% after 50h filtration with stable water flux.