Although many bioinspired superwetting materials with excellent capability for oil/water separation have been constructed, functional surfaces combining effective separation property, biodegradability, and easy-controllability are still highly desired. In this work, a facile strategy to realize the controllable wettability on the polylactic acid (PLA) nonwoven fabric has been developed; the resulting superwetting PLA nonwoven fabrics exhibit high absorption capacity and high selectivity in oil/water separation. Moreover, the superhydrophilic PLA nonwoven fabric possesses excellent simultaneous photocatalysis degradation of water-miscible toxic organic pollutants. With the versatility and biodegradability, these advanced PLA nonwoven fabrics may provide effective solutions to oily water treatment.