Carbyne is a one-dimensional allotrope of carbon consisting of a linear chain of carbon atoms bonded to each other with exceptional strength. Its outstanding mechanical, optical, and electronic properties have been theoretically predicted, but its stability has only been achieved when grown encapsulated in the hollow core of carbon nanotubes. One of the advantages of this confinement is that its properties can be controlled by the chains length and surrounding environment. We investigated an alternative way of gaining control of its properties is using isotope labelling as tuning mechanism. The optimized liquid precursor was first chosen among several options, which can greatly enhance the yield of the confined carbyne. Then isotopic labelled liquid precursor was encapsulated for further synthesis of isotopic labelled confined carbyne. This allowed us to obtain pioneering results on isotope engineered carbyne with around 11.9 % of 13 Clabelling using 13 C-methanol as precursor.Linear carbon chains (LCCs) are one-dimensional (1D) arrangements with excellent predicted mechanical, optical, and electronic properties. [1][2][3][4][5][6][7][8][9] They represent the forerunner for the true 1D carbon allotrope carbyne, an infinite or very long linear carbon chain with anticipated strength, elastic modulus, and stiffness greater than those of any known material. [10][11][12] Recently, confined carbyne (CC) was reported as the strongest known Raman scatterer with a resonant differential Raman cross section per atom in the order of 10 À22 cm 2 sr À1 , which is three orders of magnitude larger than that of any other existing material. Compared to graphene,