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The interparticle spacing of a heterostructure is a crucial factor affecting electron transfer (ET) process. Herein, binary nanoparticle superlattices (BNSLs) composed of CdSe/ZnS quantum dots (QDs) and Au nanoclusters (NCs) are prepared. Steady‐state and time‐resolved spectra illustrate that the ET accelerates as the pressure increases because pressure effectively adjusts the interparticle spacing...