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The hybrid surface expresses thermo-responsive properties and serves as a pattern to perfectly align and control the assembly of inorganic particles at the nanoscale.The vapor-liquid-solid (VLS) method is vastly employed to grow hierarchical structures with unique properties. However, key questions remain, such as what controls the branched structures and what the roles of the catalyst droplet size are during the growth. Here, an in-depth understanding of the kinetics of the nucleation, growth, and subsequent coalescence processes of Bi