Mechanochemistry has rapidly developed from a curiosity in solid-state synthesis into a powerful platform for sustainable inorganic chemistry. In main-group chemistry, ball milling provides access to molecular complexes under solvent-free or low-solvent conditions, often enabling efficient synthesis while reducing solvent consumption, reaction times, and processing demands compared with conventional solution methods. In this presentation, recent work using mechanochemistry as a versatile tool for the synthesis of main-group molecular compounds and the development of main-group mechanocatalytic processes for the conversion of CO₂ into value-added cyclic carbonate products. By connecting the synthesis of discrete main-group complexes with CO₂ activation and catalytic applications, this work illustrates how mechanochemistry can serve not only as a greener synthetic method, but also as a versatile platform fornew inorganic reactivity and advancing more sustainable chemical manufacturing.