Tree-based intercropping is considered to be a potentially useful land use system for mitigating negative environmental impacts from intensive agriculture such as nutrient leaching and greenhouse gas emissions. Rapid early growth of trees is critical for rapidly accruing environmental benefits provided by the trees. We tested the hypothesis that intercropping increases the growth and nutrient status of young hybrid poplars (Populus spp.), compared to a harrowing alley treatment (i.e., no intercrop), in two experimental sites (St-Rémi and St-Edouard) in southern Québec, Canada. Three hybrid poplar clones (TD3230, Populus trichocarpa x deltoides; DN3308, P. deltoides x nigra; and NM3729, P. nigra x maximowiczii) were planted at St-Rémi. Clones DN3333 and DN3570 were planted at St-Edouard. At St-Rémi, intercropping comprised a 4-year succession of three crops of soybean (Glycine max (L.) Merr.) and barley (Hordeum vulgare L.). At St-Edouard, intercropping comprised a 3-year succession of buckwheat (Fagopyrum esculentum Moench), winter rye (Secale cereale L.), and winter wheat (Triticum aestivum L.). At St-Rémi, four years after treatment began, leafless aboveground biomass of hybrid poplars in the intercropping treatment was 37% higher compared to that in the harrowing treatment. At St-Edouard, after the third growing season, leafless aboveground biomass of hybrid poplars in the intercropping treatment was significantly higher by 40%. Vector analysis of foliar nutrient concentrations and comparison with critical concentration values showed that N (both sites) and K (St-Edouard) were the most limiting nutrients. Hybrid poplar clones responded similarly to treatments, with no consistent differences in tree growth observed between clones. We conclude that tree-based intercropping systems may offer an effective means of improving the early growth of hybrid poplars planted to provide both environmental services and high-value timber.