Realizing programmable assembly and reconfiguration of small objects holds promise for technologically-significant applications in such fields as micromechanical systems, biomedical devices, and metamaterials. Although capillary forces have been successfully explored to assemble objects with specific shapes into ordered structures on the liquid surface, reconfiguring these assembled structures on demand remains a challenge. Here we report a strategy, bioinspired by Anurida maritima, to actively reconfigure assembled structures with well-defined selectivity, directionality, robustness, and restorability. This approach, taking advantage of optocapillarity induced by photodeformation of floating liquid crystal polymer actuators, not only achieves programmable and reconfigurable two-dimensional assembly, but also uniquely enables the formation of three-dimensional structures with tunable architectures and topologies across multiple fluid interfaces. This work demonstrates a versatile approach to tailor capillary interaction by optics, as well as a straightforward bottom-up fabrication platform for a wide range of applications.