Gas-phase curium organometallic ions were synthesized by metal/polymer co-ablation. Vacuum laser ablation of a dilute dispersion of curium oxide in polyimide resulted in several organocurium ions, evidently formed by nucleation of Cm+ and various neutral polymer fragment radicals in the ablation plume. The compositions and abundances of simple species, such as CmC2+, CmC2H+, and CmCN+, can be rationalized on the basis of the electronic structure and energetics of the curium ion, Cm+. The results for curium are in accord with a general thermochemical model previously employed to understand the organometallic speciation of preceding actinides. The identification of the above-specified species, along with several larger organocurium ions, extends the realm of organoactinide chemistry; specifically, it represents identification of a series of unique curium complexes which presumably incorporate substantially covalent (σ) Cm−C bonding. Also identified in the ablation plume were small clusters incorporating two or three curium atoms. Simple clusters, such as Cm3O4+, reveal a trivalent, lanthanide-like character for curium and reflect the tendency toward bulk, solid-state chemical behavior upon coalescence of only a few atoms. Finally, a notable ancillary observation was the formation of several clusters in which C2 evidently substituted sequentially for an O atom, revealing the pseudo-oxygen character of the dicarbide moiety.