Abstract: | Engineering synthetic materials that mimic the complex rhythmic oscillatory behavior of living cells is a fundamental challenge in science and technology. Up to now, the reported synthetic model system still cannot compete with nature in oscillatory modes and amplitudes. Presented here is a novel alternating copolymer vesicle that exhibits drastic and multimode shape oscillations in real time, which are controlled by polymer concentrations and driven by the Belousov—Zhabotinsky oscillatory reaction, including swelling/deswelling, twisting/detwisting, stretching/shrinking, fusion/fission, and multiple division. Some of them, especially the fission oscillation, have not been observed before. In addition, the oscillation magnitude with regard to diameter is much larger than that of previously reported self‐oscillating vesicles. Such a self‐oscillating vesicle transformer would extend the complexity and capacity of membrane deformations in synthetic systems, approaching those of natural cells. |