Combining infrared reflectivity, transport, susceptibility and several diffraction techniques, we find compelling evidence that CaCrO3 is a rare case of a metallic and antiferromagnetic transitionmetal oxide with a three-dimensional electronic structure. LSDA calculations correctly describe the metallic behavior as well as the anisotropic magnetic ordering pattern of C type: The high Cr valence state induces via sizeable pd hybridization remarkably strong next-nearest neighbor interactions stabilizing this ordering. The subtle balance of magnetic interactions gives rise to magneto-elastic coupling, explaining pronounced structural anomalies observed at the magnetic ordering transition.Strongly correlated electron systems including the wide class of transition-metal oxides exhibit a quite general relation between magnetic order and electrical conductivity [1]: ferromagnetism typically coexists with metallic conductivity, whereas insulators usually exhibit antiferromagnetism. It is always a challenge to understand exceptions from this rule. The rare observations of ferromagnetism in insulating transition-metal oxides most often are due to a particular type of orbital ordering [2]. The few examples of antiferromagnetic (AFM) metals, e.g., (La/Sr) 3 Mn 2 O 7 [3] or Ca 3 Ru 2 O 7 [4], are characterized by reduced electronic and structural dimensionality, and the antiferromagnetic order corresponds to a stacking of ferromagnetic (FM) layers. Here we report the discovery of a three-dimensional transition-metal oxide with metallic conductivity, antiferromagnetic exchange interactions, and C-type antiferromagnetic order: the perovskite CaCrO 3 .Perovskites containing Cr 4+ (CaCrO 3 , SrCrO 3 , and PbCrO 3 ) were already studied previously [5,6,7,8,9,10], but neither the details of the crystal structure nor the nature of the magnetic ordering are known. Only very recently evidence for C-type AFM order was reported in multi-phase samples of SrCrO 3 [10]. Regarding the conductivity, the existing data are controversial. In Refs. [7,9] CaCrO 3 was claimed to be metallic, but more recently insulating behavior has been reported [5]. A similar controversy persists also for SrCrO 3 , which should definitely be more metallic than CaCrO 3 due to the less distorted crystal structure, but metallic behavior was observed in Ref.[5] only under pressure. These controversies most likely are connected with the difficulty to prepare high-quality stoichiometric materials and with the lack of large single crystals.CaCrO 3 exhibits an orthorhombic GdFeO 3 -type perovskite structure and early magnetization measurements indicate a magnetic transition at 90 K [8], which is confirmed in our samples. Two electrons occupy the Cr 3d shell (S=1), rendering the material electronically similar to insulating RVO 3 [11] (also 3d 2 ) and to metallic (Ca/Sr)RuO 3 (4d 2 ) [12]. CaCrO 3 shows an unusually high transition-metal valence, Cr 4+ , which may lead to a small or even negative charge-transfer gap [13,14], i.e., holes in the O band. In CrO 2 with ruti...