Climate-induced changes contribute to the thawing of ice-rich permafrost in the Arctic, which leads to the release of large volumes of organic carbon into the atmosphere in the form of greenhouse gases, mainly carbon dioxide and methane. Ground ice constitutes a considerable volume of the cryogenically sequestered labile dissolved organic carbon (DOC) subjected to fast mineralization upon thawing. In this work we collected an unique geochemical database of the ground and glacier ice comprising the samples from various geographic locations characterized by a variety of key parameters, including ion composition, carbon-bearing gases (methane and carbon dioxide) bulk biogeochemical indicators and fluorescent dissolved organic matter (DOM) fractions. Our results show that interaction with solid material—such as sediments, detritus, and vegetation—is likely the overriding process in enrichment of the ground ice in all the dissolved compounds. Terrigenous humic-like dissolved organic matter was predominant in all the analyzed ice samples except for glacier ice and pure tabular ground ice from Mare Sale (Western Yamal). The labile protein-like DOM, indicating an autochthonous source, showed no correlation to humic components and probably associated with microbial abundance in the ground ice. The sum of the fluorescent DOM components satisfactory correlates to DOC, indicating the adequacy of the estimation. The pure tabular ground ice samples exhibit the highest biogeochemical quality which may be responsible for the amplification of permafrost organic matter decomposition upon thawing. Yamal impure tabular ground ice and ice wedges are extremely enriched in methane compared to the samples from other locations which should cause a portion of direct methane emission upon the putative thawing.