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We report the fabrication of multi-island single-electron devices made by lithographic contacting of self-assembled alkanethiol-coated gold nanocrystals. The advantages of this method, which bridges the dimensional gap between lithographic and NC sizes, are (1) the fact that all tunnel junctions are defined by self-assembly rather than lithography and (2) the high ratio of gate capacitance to total capacitance. The rich electronic behavior of a double-island device, measured at 4.2 K, is predicted by combining finite element and Monte Carlo simulations, and it can be fully explained by the standard theory of Coulomb blockade with very few adjustable parameters.© 2006 American