It was recently shown that nanostructured targets with largely spaced gold ultrasmall nanoparticles (NPs) show outstanding performances in enhancing the laser-driven ions' acceleration process due to the higher laser-to-target energy absorption [Vallières et al., Phys. Rev. Accel. Beams 22, 091303 (2019)]. Based on this structure, here, an alternative nanostructured design is proposed to promote light/heavy ions' acceleration quality. The scheme relies on using a gold NP layered nanosphere filled with a low-density argon gas. The nanosphere has an inner layer of vanadium and an outer layer of proton–carbon (1:1) mixture. The validity of this suggestion has been simulated by the two-dimensional particle-in-cell code (EPOCH). Simulation results indicate that the interaction of ultra-intense laser (∼4.61 × 1019 W/cm2) with a gas-filled gold NP layered nanosphere can positively decrease the aggregation of electrons stated inside the target, leading to higher Coulomb repulsion between charged ions. Therefore, we can expect the generation of quasi-monoenergetic H+, C6+, V20+, and Au49+, as well as Ar15+ (cutoff energy of ∼0.49 MeV/u and relative divergence angle of 2.9°) at the end of the interaction. From simulations, as the interaction terminates, for a gas-filled gold NP layered nanosphere with an optimal gap space of 80 nm, a cutoff energy increase of roughly 19% for H+, 16.4% for C6+, and rather equal percent of 15.9% for medium-heavy ions (V20+ and Au49+) is obtained with respect to a hollow gold NP layered nanosphere. Moreover, a relative divergence angle decrease of up to nearly 0.29–1.91 times will be calculated for the accelerated ions. Overall, the results verify that a gas-filled gold NP layered nanosphere can be regarded as a candidate for the generation of quasi-monoenergetic ions through the spherical Coulomb explosion regime.