In recent years, the problem of oily sewage has seriously affected the ecological environment and human health. Thus, we prepared a novel biodegradable poly (lactic acid) (PLA) membrane with antibacterial property and oil–water separation function via electrospinning method. First, the matter of silver ion glass microbeads (AgGB) loaded with layered double hydroxides (LDHs) and the LDH@AgGB modified with 3‐triethoxysilyl‐1‐Propanamine (APTES) were synthesized. Then, the LDH@AgGB were blended with PLA to prepare PLA/LDH@AgGB composite. And the PLA nanofibrous membranes were electrospun. The results showed that APTES could significantly improve the dispersion and compatibility of LDH@AgGB in PLA matrix. The addition of A‐LDH@AgGB could greatly improve the crystallinity, and control the porosity and pore‐size of PLA membranes. The maximum water contact angle of the PLA membranes could reach to 109.31°, while the oil contact angle of the PLA membranes decreased to 0° resulting in a high oil absorption capacity, and fast oil absorption rate performance. Meanwhile, the PLA membrane had efficient antibacterial property against Escherichia coli. The reported novel LDH@AgGB and its PLA composite membrane provided a method for designing and preparing environmental‐friendly, high‐performance materials with both excellent antibacterial property and oil–water separation.

Controlling wettability is crucial to designing separation membrane with high performance. In order to achieve the goal, chain modification method is frequently utilized to optimize surface nature of raw materials. However, the development of the method is of significance but challenging due to the high processing cost and complexity. Herein, we developed a rough surface induction strategy to prepare poly(lactic acid) (PLA) membrane. Layered double hydroxides (LDH) were loaded with carboxylation carbon nanotubes (CNT), and the prepared CNT@LDH was surface modified with aminopropyltriethoxysilane. Then the CNT@LDH was blended with PLA to prepare composites and PLA electrospinning membranes. The morphology of synthesized CNT@LDH mimics "sea urchin" liked structure, which prevented the aggregation of LDH cubes, and induced an efficient conductive network. The combination of CNT@LDH greatly changed the membranes' porous structure, thermal stability, and crystallization properties. The hydrophilicity of PLA membranes increased 112.74%, whereas the pore size and fiber diameter decreased 76.43% and 79.56%, respectively. The oil absorption capacity of the composite membrane was up to 35 g/g with a high absorption speed. Meanwhile, the prepared PLA membrane had a quick response of press-sensing.This research provides a method for designing separation membranes with high separation efficiency, great selectivity, environment friendliness, and realtime pressure monitor function, which is considered as a potential material in intelligent oil-water separation or wearable electronics fields.