Over the past two decades, advances in modern biology and nanotechnology have enabled a rapid development in the design and building of biomimetic functional materials. ATP synthase is one of the most extensively studied molecular machines because it can be used as a rotary motor in the design of novel nanodevices and it can also continuously synthesize ATP in an artificial environment. A lot of research efforts have focused on assembling ATP synthase in biomimetic systems so that a complex cellular process can be constructed in a controllable manner. As we summarize here, layer-by-layer assembled microcapsules have proved to be a suitable cellular mimetic structure, which can be applied for engineering active biomimetic systems with a cellular process. An added benefit is that these assembled microcapsules can be used as bioenergy containers and thus ATP supply on demand.