Poly(lactic acid) (PLA), one of the most promising biodegradable polymer products, has achieved wide applications for its relatively good mechanical properties and moderate degradability. Here we report an environment-friendly filler, the organic-inorganic composite Janus nanosheets (PLA/PBS JNs), which can jam at the interface of the PLA/PBS blend with a low threshold as the compatibilizer and can simultaneously toughen the composites and improve the gas barrier performance due to better interfacial interaction and tortuous path effect. With 0.3 wt % of PLA/PBS JNs added, the tensile strength and elongation at break of the PLA/PBS blend can be improved by 37% and 224%, respectively. After a further hot-pressing process, the barrier performance of the PLA/PBS composite membranes can be significantly enhanced since PLA, PLA/PBS JNs, and PBS are arranged in a nearly lamellar structure with oxygen permeability of 0.63 × 10-15 cm3 cm·cm-2 s-1 Pa-1 with only 0.5 wt % of PLA/PBS JNs.