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Infrared emission bands with wavelengths between 3-20 {\mu}m are observed ina variety of astrophysical environments [1,2]. They were discovered in the1970s and are generally attributed to organic compounds [3,4]. However, over 40years of research efforts still leave the source of these emission bandslargely unidentified [5-7]. Here, we report the first laboratory infrared (6-25{\mu}m) spectra of gas-phase fullerene-metal complexes, [C60-Metal]+ (Metal =Fe and V), and show with density functional theory calculations that complexesof C60 with cosmically abundant metals, including Li, Na, K, Mg, Ca, Al, V, andFe, all have similar infrared spectral patterns. Comparison with observationalinfrared spectra from several fullerene-rich planetary nebulae demonstrates astrong positive linear cross-correlation. The infrared features of [C60-Metal]+coincide with four bands attributed earlier to neutral C60 bands, and inaddition also with several to date unexplained bands. Abundance and collisiontheory estimates furthermore indicate that [C60-Metal]+ could plausibly formand survive in astrophysical environments. Hence, [C60-Metal]+ are proposed aspromising carriers, in supplement to C60, of astronomical infrared emissionbands, potentially representing the largest molecular species in space otherthan the bare fullerenes C60, C60+, and C70. This work opens a new chapter forstudying cosmic fullerene species and carbon chemistry in the Universe.

Buckyball-metal complexes as promising carriers of astronomical unidentified infrared emission bands