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Our work demonstrates that ultrathin freestanding films can exhibit functional properties that are absent in homogeneous materials, concomitant with their convenient compatibility with Si-based devices.We report the synthesis of all-frame-faceted octahedral nanoframes containing eight Y-shaped hot zones in a single entity where electromagnetic near-field focusing can be maximized. To realize such state-of-the-art complex nanoframes, a series of multiple stepwise bottom-up processes were executed by exploiting Au octahedral nanoparticles a