Chaotic systems comprising of active materials have the capability to absorb energy directly from the external environment to preserve their own sustained motion, holding tremendous potential for utilization in diverse fields, for instance, controllable sensors, energy harvesting, motion behavior control of smart materials and more. In this paper, a sustained jumping system consisting of photosensitive liquid crystal elastomer (LCE) balloon is developed innovatively, in which the LCE balloon can transition from a static state to a sustained jumping state under periodic illumination. Given the dynamic constitutive model of LCE and Hertz contact theory, the nonlinear dynamics model of the sustained jumping LCE balloon system is established. Numerical calculations demonstrate the existence of two jumping modes for the LCE balloon, i.e., periodic jumping and chaotic jumping. The mechanism of sustained jumping that counterbalances the energy dissipation by the net work combining contact expansion and buoyancy variation, as well as the mechanism of chaotic phenomena, are revealed. In addition, the influences of vital parameters on the jumping mode of the balloon are examined, and the conversion of the jumping modes with parameters is illustrated by bifurcation diagrams. This work can broaden the knowledge of the dynamic behavior of smart materials, which is of guiding significance for the research on chaos control and chaotic system design.