Nanomaterials, such as single‐walled carbon nanotubes (SWCNTs) and graphenes, can be readily gelled using bi‐ or multi‐functional reagents as crosslinkers. This study reports a new reaction of monofunctional acetylenes with negatively charged SWCNTs (nanotubides), prepared by reduction. Mono‐acetylenes (e. g. phenylacetylene (PAc) and diphenyl acetylene (DiPAc)) are introduced as crosslinkers to form all‐carbon SWCNT organogels at room temperature. The resulting isolated SWCNT aerogels have a density of ∼4.5–5.5 mg cm−3. Raman spectroscopy and thermogravimetric analysis suggest a covalent surface modification (∼1 functional group per 110 (PAc) and 712 (DiPAc) SWCNT carbon atoms). Significantly, the acetylene reaction does not consume all available negative charges. The SWCNT organogel is still reactive after crosslinking and can reduce a stable gold complex, chloro(triphenylphosphine)gold (I), to form AuNPs (∼12–14 nm), suggesting the formation of a living nanotubide organogel intermediate, suitable for a range of secondary reactions. Mono‐acetylenes can crosslink other negatively charged molecular systems, and surface decoration of the aerogels with other metal NPs is anticipated.