Many complex biological and technological systems can be represented by multilayer networks where the nodes are coupled via several independent networks. Despite its significance from both the theoretical and the application perspectives, synchronization in multilayer networks and its dependence on the network topology remain poorly understood. In this talk, we will present a universal connection graph-based method which opens up the possibility of explicitly assessing critical multilayer-induced interactions which can hamper network synchronization. The method reveals striking, counterintuitive effects caused by multilayer coupling. It demonstrates that a coupling which is favorable to synchronization in single-layer networks can reverse its role and destabilize synchronization when used in a multilayer network. This property is controlled by the traffic load on a given edge when the replacement of a lightly loaded edge in one layer with a coupling from another layer can promote synchronization, but a similar replacement of a highly loaded edge can break synchronization, forcing a "good" link to go "bad." We will also discuss open problems and challenges in studying cooperative dynamics of multilayer networks.