Optically left-handed materials refract the propagating light in the opposite direction. Most research has focused on the design of various structures, including split-ring resonators, either on planes or in particle cluster forms to resonate with specific light frequencies. However, for particle-based materials, the circuital structures for optical left-handedness have not been fully understood and the effect of interior structure on the optical handedness have not been investigated. Additionally, scalable methods to deploy the unique characteristics of the materials have not been reported so far and are still urgent. Here, optically left-handed nanopearl beads are synthesized in up to 1.25 L solutions. Nanopearl beads contain assembled Au nanocolloids, a dielectric sphere, and a thin silica layer that fixes the assembled structures to sustainably yield unique inductance-capacitance circuits at specific visible-near-infrared frequencies. The frequencies are tunable by modulating the interior structures. Investigation of the circuit structures and Poynting vectors generated within the nanopearl beads suggest the likelihood of their left-handedness. Moreover, the effects of interior structures on the optical handedness of the nanopearl beads are extensively investigated. The results could help commercialize optically left-handed materials and pioneer fields that have not been realized so far.