Bond activation and catalysis are central to the development of a sustainable energy system. Frustrated Lewis Pairs have conceptually revolutionized the activation of inert chemical bonds. Far less developed are hybrid systems containing at least one transition metal as part of the electron-donating/accepting composition. These cooperative transition metal architectures present advantages over traditional systems. For instance, they incorporate, to the concept of FLPs, the movement of electron pairs as typically encountered in the elementary steps of organometallic catalysis. This Perspective presents arguably the most relevant and recent progress of a vivid field of research that aspires to implement cooperative designs in polarized transition metal systems. Moreover, it provides tools for future developments and shows that molecular control over bond-making and -breaking processes can be achieved.

Reduction of LPhSnCl with 0.66 eq. of LiBsBu3H affords the mixed-valent homocatenated tri-tin complex (LPhSn)3Cl whose HOMO primarily comprises σ-bonding along the Sn–Sn–Sn framework.

Future chemicals should preserve the efficiency of their function while reducing hazards and waste. In this context, catalysis – a fundamental pillar of Green Chemistry – is still the most effective technique capable of meeting societal requirements while offering sustainability. To further push the boundaries of catalysis and respond to these challenges, a clear understanding of the molecular level interactions is essential. To succeed, we believe it is necessary to consider the transition metal catalyst as a molecular system encompassing a local and non‐local environment. The synergistic effects that are taking place between the ligand, the metal center, and their surrounding environments primarily determine the efficiency of the bond making and breaking processes. This Concept provides tools for identifying, implementing, and combining these effects to control catalysis directly at a molecular level.