systems have been known very early; however, in vitro mimicking such "living" systems with adaptive features using "nonliving" molecular building blocks is still a fundamental challenge in chemistry. [5,6] To date, chemists have established a plethora of synthetic self-assembly entities, [7] some of which can undergo reversible shape changes or phase transitions under external stimuli, [8][9][10] but they are not yet comparable to their natural counterparts. The main reason is that synthetic self-assembly systems operate in thermodynamic equilibrium, resulting in timeindependent steady-state structures. In contrast, natural self-assembly requires a continuous supply of energy to keep the assemblies away from equilibrium, resulting in time-dependent dynamic structures. [11] If the energy dissipates, the system will fall apart and revert to ground state. This process is referred to as dissipative self-assembly, [12] which offers impetus for biological motions such as cell deformation and growth (in situ motion without distance change), and cell migration and division (motion with distance change). Hence, implanting this energy-driven assembly in man-made assemblies may create life-like systems, possessing structural adaption and behavioral evolution over time and space. However, such artificial systems formed by dissipative pathway are quite limited thus far. The few reports focused on biocatalytic active gels, [13][14][15] switchable films, [16] and molecule-level reaction networks. [17] Nanoscale nonequilibrium assemblies have received little attention. An insuperable obstacle is how to harmonize sophisticated self-assembly process with continuous energy influx in a time-ordered manner.Herein, we report a "living" giant vesicle system that can perform autonomous and periodic pulsating motion via energy dissipation. The energy source of this pulsation derives from the cellular biochemical fuel, ATP. To achieve the energy-regulated self-assembly, our design concept is based on transient ligandreceptor supramolecular interactions between the ATP fuels and the vesicular membrane components. The system is necessary to satisfy the following conditions: (i) a self-assembling vesicle with specific ATP receptor units can toggle between expansile and contractile state by the association and dissociation of ATP; (ii) the temporary formation of ATP-polymer ligand-receptor complexes can cause the system energy gain Living systems can experience time-dependent dynamic self-assembly for periodic, adaptive behavior via energy dissipation pathway. Creating in vitro mimics is a daunting mission. Here a "living" giant vesicle system that can perform a periodic pulsating motion using adenosine-5'-triphosphate (ATP)-fuelled dissipative self-assembly is described. This dynamic system is built on transient supramolecular interactions between the polymer and cellular energy currency ATP. The vesicles capturing ATPs will deviate away from equilibrium, leading to an energy ascent that drives a continuous vesicular expansion, until a comp...