In this article, we examine the reactions between methane molecules as a starting point for hydrocarbon growth in space and assess the effectiveness of the ion−ion reaction between CH 4 + and CH 4 + using quantum mechanical and molecular dynamics methods. We modeled the reaction starting from the dicationically ionized [CH 4 •••CH 4 ] 2+ cluster. Initially, attractive interactions occur between the facing C−H bonds of the tetrahedral structures, which are electron-deficient. As the structure transitions to a trigonal pyramid, a bond begins to form between two carbon atoms with unpaired electrons, resulting in a metastable configuration due to the balance between Coulombic repulsion and attractive forces. The stabilization energy for C−C bond formation was 176.8 kcal/mol, with a bond formation efficiency of 32.6%, and the corresponding rate coefficient was 1.394 × 10 −2 fs −1 . This stabilization by C−C bond formation generates kinetic energy, and if sufficient energy is redistributed to the vibrational mode of the reaction, the reaction can proceed. Reactions involving C−C bond formation produced precursors of ethane, ethylene, and acetylene, such as C 2 H 6 2+ , C 2 H 5 + , C 2 H 4 + , and C 2 H 3 + , as well as CH 3 + , a key species in ion− molecule reactions in space. Even without C−C bond formation, a significant amount of CH 3 + was produced. Our findings underscore the importance of exploring novel ion−ion reactions to deepen our understanding of molecular growth in space. KEYWORDS: hydrocarbon molecular growth in space, ion−ion reactions of methane, driving force of reactions, energy redistribution, quantum mechanical methods, molecular dynamics methods