Solar geoengineering and negative-emissions technologies are attracting greater attention as prospective ways to tackle and mitigate the worst impacts of climate change. Until now, such options have rarely been examined in a comprehensive manner. Rather, insofar as this has been done, research focused on one or the other, rather than considering a portfolio contribution and, more often, has taken a sectoral approach that looks at the options germane to the agriculture or energy sectors, but not in relation to climate change. Arguing for the need for a wider lens, the current article aims to understand the kinds of couplings and linkages most germane for the effectiveness of a particular option. In specific, we employed a novel dataset garnered from a large expert-interview exercise (N = 125) to conceptualize and consider crucial couplings to solar radiation management and carbon dioxide removal at many levels (across different sectors, differing dimensions of sustainability, productive or destructive impacts, and direct and indirect relationships). Our analysis thereby provides insights into the understanding of climate transitions by explicitly considering the most salient couplings in general as well as how, and to what extent, the various options relate to each other, as a portfolio for climate intervention, and together to climate mitigation and adaptation.