Sulfide- and sulfate-rich hydrothermal vents are involved in Earth's major geochemical cycles. An outstanding scientific question consists of finding out whether certain minerals found in hydrothermal chimneys are influenced more or less directly by microorganisms living at high temperatures (thermophiles or hyperthermophiles) in these environments. Here we report the morphological, textural and chemical characterization of pyrite crystals collected across a section of a chimney from the Trans-Atlantic Geotraverse hydrothermal site, sampled from the inner, hotter portion to the external, cooler portion, providing a promising approach to the search for hyperthermophilic biosignatures. The internal and middle portions of the chimney mainly harbour cube-shaped pyrite containing low quantities of hydrocarbons and thermally matured organic compounds. In contrast, the samples from the external portion contain pyrite spherules composed of a mosaic of slightly disoriented domains that include large amounts of organic material chemically consistent with thermally matured biogenic organic compounds. These characteristics make them comparable but not identical to pyrite spherules produced in the laboratory in the presence of hyperthermophilic archaea of the order Thermococcales. Differences include larger crystalline domains and more thermally matured organic compounds. Such features could be consistent with the thermal transformation of pyrite spherules produced by (or at least in the presence of) living cells. However, it remains impossible to completely rule out an abiotic origin without further isotopic investigation and experimental studies on the abiotic production of pyrite spherules in the presence of organic compounds and under hydrothermal conditions.