During the last 5 years, laboratory experiments relevant to the formation of carbon-bearing molecules in extraterrestrial environments have been performed employing the crossed molecular beam technique and a high intensity source of ground state atomic carbon, C(3
). These investigations unraveled for the first time detailed information on the chemical reaction dynamics, involved collision complexes and intermediates, and – most important – reaction products of neutral-neutral reactions. Here, we extend these studies even further, and report on very recent crossed beam experiments of cyano radical, CN(2Σ+), reactions with unsaturated hydrocarbons to form nitriles in extraterrestrial environments and Saturn's moon Titan. Further, preliminary results on reactions of small carbon clusters and with acetylene, ethylene, and methylacetylene to synthesize hydrogen-deficient carbon-bearing molecules are presented.