Combating climate change and achieving the UN Sustainable Development Goals (SDGs) are two important challenges facing humanity. Natural climate solutions (NCSs) can contribute to the achievement of these two commitments but can also generate conflicting trade-offs. Here, we reviewed the literature and drew on expert knowledge to assess the co-benefits of and trade-offs between 150 SDG targets and NCSs within 12 selected ecosystems. We demonstrate that terrestrial, coastal, and marine NCSs enable the attainment of different sets of SDG targets, with low redundancy. Implementing NCSs in various ecosystems would therefore maximize achievement of SDG targets but would also induce trade-offs, particularly if best practices are not followed. Reliance on NCSs at large scales will require that these trade-offs be taken into consideration to ensure the simultaneous realization of positive climate outcomes and multiple SDG targets for diverse stakeholders.