Efficient removal of trace amounts of dissolved organics with moderate polarity (DOMP) in water via adsorption method is a challenge. Most typical adsorption materials such as activated carbon exhibits poor selectivity and few polymers can remove DOMP in water. Herein, four polyacrylate resin (PAR)-based materials with different side chain are successfully fabricated, which can selectively adsorb pure organics with moderate polarity (dielectric constant ranging from 2.21 to 21). Interestingly, PARs can also selectively remove low concentration of toluene (5 ppm) and chloroform (1 ppm) in water with maximum removal efficiencies of 98.16% and 95.65%, respectively. Molecular dynamic (MD) simulations reveals that the driving force and selectivity of the adsorption behaviors can be attributed to the van der Waals interactions between the side chain of PARs and organics. Our study provides a designing strategy and novel material for efficient removal of organic pollutants with trace amounts in water.