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Bifunctional molecules can be used to tether quantum dots to nanostructured and planar semiconductor and metal surfaces. Excited-state interfacial electron-transfer reactions at QD−molecule−substrate interfaces are of interest from a fundamental standpoint and may have applications in solar energy conversion and charge-transfer-based sensing. This Perspective highlights recent work and unanswered questions in two related areas, the linker-assisted assembly of QD−substrate architectures and the spectroscopic characterization of electron transfer at QD−molecule−substrate interfaces.