The realization of high-yield, stable molecular junctions has been a long-standing challenge in the field of molecular electronics research, and it is an essential prerequisite for characterizing and understanding the charge transport properties of molecular junctions prior to their device applications. Here, we introduce a new approach for obtaining high-yield, vertically structured metal-molecule-metal junctions in which the top metal electrodes are formed on alkanethiolate self-assembled monolayers by a direct metal transfer method without the use of any additional protecting interlayers in the junctions. The fabricated alkanethiolate molecular devices exhibited considerably improved device yields (∼70%) in comparison to the typical low device yields (less than a few %) of molecular junctions in which the top metal electrodes are fabricated using the conventional evaporation method. We compared our method with other molecular device fabrication methods in terms of charge transport parameters. This study suggests a potential new device platform for realizing robust, high-yield molecular junctions and investigating the electronic properties of devices.