The development of frustrated Lewis pairs (FLPs) and their application in bond activation and catalysis have emerged as a hot topic in the field of main group chemistry over the last two decades. The introduction of metals into these systems has become a turning point in this area due to their potential to overcome the main limitations of main group elements in catalysis. Herein, we have tried to summarize the most relevant results in which metals play a key role in these cooperative systems. The main aim of this chapter focuses on describing the cooperative modes of activation between the metallic Lewis acidic and basic partners of the FLP architectures to illustrate the vast opportunities that the combination of two metal centers presents. In addition, we have introduced several bimetallic systems which may not be strictly considered as FLPs, but their strong structural and reactive similarities are helpful to understand and showcase the intricacies of bimetallic cooperation.