<abstract abstract-type="main" xml:lang="en"> <title>Abstract</title> <p>Reaction of tetrakis(trimethylsilyl)tetrahedrane with MeLi produces a solution of tris(trimethylsilyl)tetrahydryl lithium which is easily amenable for Pd‐catalyzed cross‐coupling processes to produce thermally stable arylated tetrahedranes.</p> </abstract>