A sandwich architecture including double crystal substrates and a single glass-forming droplet has been successfully designed based on the simplified liquid-bridge methods in multicomponent alloys. The multiscale precipitates mainly consisting of β-phase dendrites with a body-centered cubic (BCC) structure, cubic CuZr2 phase, and icosahedral quasicrystalline phase (I-phase) could be simultaneously identified in dissimilar regions of the glass-forming matrix during heat-induced dissolution or diffusion from crystal substrate to glass-forming droplet. The gradient distributions of crystal-like clusters not only accelerate diffusion velocity due to the collective atomic motion but also can simultaneously modulate the atomic-scale structure, mechanical response, and chemical composition via tracing a high-throughput strategy. The present work provides new insights to discover the formation mechanism of the representative microstructures strongly associated with the atomic-scale structure-property-composition relationships and is also helpful to shed light on the in-situ origin or structural mechanism of supercluster-induced multiscale precipitates in developing bulk metallic glasses (BMGs) and in-situ formed BMG composites (BMGCs).