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Heterobimetallic cationic sandwich complexes [M(μ‐Cp)M′Cp] +  of group 13 (M=Ga, In) and group 14 (M′=Ge, Sn) elements have been prepared as [WCA] −  salts (WCA=Al(OR F ) 4 ; OR F =OC(CF 3 ) 3 ). Their molecular structures include free apical gallium or indium atoms. The sandwich complexes were formed in the reactions of [M(HMB)] + [WCA] −  (HMB=C 6 Me 6 ) with the free metallocenes [M′Cp 2 ]. Their structures are related to known stannocene and stannocenium salts; the unprecedented germanium analogues, namely the free germanocenium cation [GeCp] +  and the corresponding triple‐decker complex cation [CpGe(μ‐Cp)GeCp] + , are described herein. By variation of the reaction conditions, these sandwich complexes can be transformed into the group 13/14 mixed cationic coordination polymer [{In(HMB)(μ‐SnCp 2 )}  n  ][WCA]  n  . This polymeric chain motif was also successfully replicated by the synthesis of complexes [{Ga/In(HMB)(μ‐FeCp 2 )}  n  ][WCA]  n   containing FeCp 2  as a bridging ligand.

Stack by Stack: From the Free Cyclopentadienylgermanium Cation Via Heterobimetallic Main‐Group Sandwiches to Main‐Group Sandwich Coordination Polymers