Metallofoldamers are sequence‐specific oligomers, which are designed to fold into three‐dimensional architectures upon metal coordination. Their folding can involve additional noncovalent interactions and results in new chiral secondary structures, enhanced stabilization of existing secondary structures, or unique materials for specific applications. This microreview highlights recent advances in the field.(© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2009)