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Cruciform-like molecules with two orthogonally placed conjugated systems have in recent years attracted significant interest for their potential use as molecular wires in Molecular Electronics. Here we present a large selection of cruciform molecules based on oligo(phenyleneethynylene) (OPE) and tetrathiafulvalene (TTF) scaffolds, end-capped with acetyl-protected thiolates as electrode anchoring groups [1,2].