Due to its rough, mountainous relief, Samothraki remains one of the last minimally disturbed islands in the Mediterranean. This paper examines the hydrogeochemical regime of the island’s surface waters as it results from geological, morphological, and hydro(geo)logical controls within a frame of minimally disturbed environmental conditions. Shallow, fractured groundwater aquifers, in combination with steep slopes and predominant weathering resistant rocks, bring about flashy stream regimes with remarkably low solute concentrations. Streams and springs revealed hydrochemical similarities. Contrary to streams chiefly draining sedimentary rocks, streams underlined by granite and ophiolite rocks do not respond hydrochemically to geochemical differences. Using ion proportions instead of concentrations, geochemical fingertips of magmatic stream basins were detected. Atmospheric inputs largely affect stream and spring composition, e.g., by 75% regarding sodium. Only 20% of dissolved oxygen and pH variance was assigned to biological activity, while nutrient levels were consistent with the undisturbed conditions of the island, except nitrate. Small mountainous springs and brooks fed by restricted, fractured groundwater aquifers with perennial flow, despite scarce summer rainfalls, may be fueled by cloud and fog condensation. High night-day stream flow differences, high atmospheric humidity predominately occurring during the night, and low stream water travel times point out toward this phenomenon.