Open-shell compounds bearing metal-carbon triple bonds, such as carbides and carbynes, are of significant interest as plausible intermediates in the reductive catenation of C1 oxygenates. Despite the abundance of closed-shell carbynes reported, open-shell variants are very limited, and an open-shell carbide has yet to be reported. Herein, we report the synthesis of the first terminal, open-shell carbide complexes, [K][1] and [1][BArF4] (1 = P2Mo(≡C:)(CO), P2 = a terphenyl diphosphine ligand), which differ by two redox states, as well as a series of related open-shell carbyne complexes. The complexes are characterized by single-crystal X-ray diffraction and NMR, EPR, and IR spectroscopies, while the electronic structures are probed by EPR studies and DFT calculations to assess spin delocalization. In the d1 complexes, the spin is primarily localized on the metal (∼55-77% Mo dxy) with delocalization on the triply bonded carbon of ∼0.05-0.09 e-. In the reduced carbide [K][1], a direct metal-arene interaction enables ancillary ligand reduction, resulting in reduced radical character on the terminal carbide (⩽0.02 e-). Reactivity studies with [K][1] reveal the formation of mixed-valent C-C coupled products at -40 °C, illustrating how productive reactivity manifolds can be engendered through the manipulation of redox states. Combined, the results inform on the electronic structure and reactivity of a new and underrepresented class of compounds with potential significance to a wide array of reactions involving open-shell species.