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By the early 1960s, several Arctic nations had begun to worry about one of the most iconic and elusive species living across and beyond their Northern territorial borders: polar bears. Following the end of WWII, white trophy hunters used new kinds of airplanes, ships, guns, and trapping devices to be able to reach and kill more of these apex predators than ever before. Alarmed by this spike in polar bear harvest, a group of politicians, conservationists, and scientists from all five Arctic nations met in Fairbanks, Alaska, in 1965. There, they decided to establish a “Polar Bear Specialist Group” under the auspices of the Switzerland-based International Union for Conservation of Nature and to launch circumpolar scientific efforts to gather new knowledge on the species in order to guide both national and international legislation. However, as this paper argues, Arctic hunting was not only the trigger but also the metaphorical bullet for a new kind of polar bear science. Based on archival records and published sources on polar bear hunting and research in Alaska, Northern Canada, Greenland, and Svalbard in the 1960s and 1970s, this paper traces how the adaption of legal and administrative frameworks of game management on the one hand and international scientific collaboration in and off the field on the other hand led to a redeployment of Arctic hunting, including its knowledges, technologies, and actants, for large-scale scientific monitoring and sampling ambitions. As part of this, scientists enrolled not only white trophy hunters to obtain data and collect biological specimens but also Indigenous subsistence hunters—though not in the same way. This paper consequently also examines the plural imaginaries and cultures of hunting and of “wildlife”-human relations in the High Arctic as they became entangled in Cold War science and conservation politics in complex and asymmetrical ways.