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The new European Union Forest Strategy for 2030 aims to plant an additional 3 billion trees on non-forest land to mitigate climate change. However, the choice of tree species for afforestation to achieve the maximum climate benefit is unclear. We compared the climate benefit of six different species in terms of carbon (C) sequestration in biomass and the harvested wood substitution in products to avoid carbon dioxide (CO₂) emissions from fossil-based materials over the 100-year period by afforesting about ¼ of the available area in northern Europe. The highest climate benefit was observed for larch, both at a stand scale (1626 Mg CO₂ eqv. ha⁻¹) and at the landscape level for the studied scenario (579 million Mg CO₂ eqv.). Larch was followed by Norway spruce, poplar, hybrid aspen and birch, showing a climate benefit about 40–50% lower than that for larch. The climate benefit of willow was about 70% lower than larch. Willow showed 6–14-fold lower C stocks at the landscape level after 100 years than other tree species. The major climate benefit over the 100-year period comes from wood substitution and avoided emissions, but C stock buildup at the landscape level also removes significant amounts of CO₂ already present in the atmosphere. The choice of tree species is important to maximize climate change mitigation.