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The paper provides a detailed overview of the scientific background, mostly published in 1970s–1990s, which resulted in tremendous success in preparation of modified electrodes, later used for bioelectrochemical, (bio)catalytic, photoelectrocatalytic, and other applications. The systems overviewed in the paper are focused on the chemisorption of sulfur-containing molecules (thiols, disulfides, sulfides, etc.). The self-assembling of these molecules at various metal (mostly Au and Pt) electrodes resulted in the formation of the well-structured monolayers, which allowed unique chemical and electrochemical features, not achievable by other modification techniques. Notably, the present paper is different from other typical reviews and books about chemically modified electrodes—it is not aimed at highlighting the recent achievements in the research area, but provides a detailed analysis of the area background produced …