Laser ablation into vacuum of a dilute dispersion of AmO2 in polyimide produced organoamericium ions of the general formula AmCxHyNz+. Ion masses were determined by time-of-flight mass spectrometry, and compositions were confidently assigned for most small ions (x less than or equal to 6). Comparisons of product abundances with previous results for lanthanides (Ln) and lighter actinides (An) suggest that Am behaves similarly to a lanthanide element such as Tm-both produced substantial MC2H+ (acetylide) and MC4H+. In contrast, the lighter actinides, Th, U, Np, and Pu, preferentially produced the binary carbides MC2+ and MC4+. The acetylides can be regarded as ionic species comprising M2+ ([M2+-{(-):C=CH}](+)) and the carbides as comprising M3+ ([M3+-{(-):C=C:(-)}](+)). Accordingly, the MC(2)H(+ )vs MC2+ abundances generally correlated with the ionization energies from M2+ to M3+ (IE[M2+]). In addition to the carbide/hydrocarbide complex ions, Am+-hydroxide, -cyanide, -cyanate, and -nitrile ions were produced in abundances generally consistent with IE[Am+] and IE[Am2+]. Both AmCN+ and AmC2H+ comprise nominally divalent Am2+, but the relative abundance of the cyanide (vs acetylide) species was greater for Am than for the preceding An, suggesting a greater degree of ionicity in the Am complexes. Larger AmCxHyNz+ were identified for x up to similar to 12, with compositions consistent with the ionic bonding model used to represent the smaller Am+-R. The formation and possible structures of the larger species are considered with regard to the neutrals produced during ablation of polyimide. In addition, substantial amounts of directly ablated fullerene ions (and neutrals), C-50(+)-C-greater than or equal to 125(+), were produced under favorable ablation conditions. An anomalously intense peak corresponding to C-110(+) is considered to probably comprise a contribution from the metallofullerene of similar mass, Am+-C-90. On the basis of the divalent character of Am, this species could be represented as Am2+-C-90(-), although the present results provide do not indicate whether such a species should be regarded as an exohedral or endohedral metallofullerene. This work extended the production of labile gas-phase organoactinide complexes to the first transplutonium element Am-this technique is applicable to highly radioactive elements not amenable to conventional methods. The results revealed the divalent character of Am not evident for the preceding An. The low-valent sigma-bonded organometallics identified in the gas phase are difficult to isolate for the lanthanide and transuranium actinide elements, but polymer ablation into vacuum accesses transient/metastable species by supplying highly reactive hydrocarbon radicals to a free metal center.