When many of today’s deepest problems are intractable, how can public, private, and nonprofit actors collaborate to mitigate negative local effects? Given the open-endedness of any collective effort to “chip away” at a grand challenge, these intersectoral collaborations must align the scope of a shared goal with the governance arrangements distributing decision-making authority. By juxtaposing insights from fieldwork on intersectoral collaborations formed to aid local homeless communities in São Paulo (Brazil), California (USA), and Manchester (UK), this research presents four goal-governance alignments to achieve coordinated collective action. To pursue a targeted goal, an organization can set up or join a local structure of centralised (Partnerships) or distributed (Coalitions) decision-making authority. To pursue broader goals, an organization can evolve into a Mission by engaging simultaneously in multiple, mutually reinforcing local partnerships and coalitions. Or evolve into a Movement by not only adding local structures of collective action, but also adopting a participation architecture to encourage collaboration at scale from third parties outside the organization’s managerial control.