World population is projected to reach over nine billion by the year 2050, and ensuring food security while mitigating environmental impacts represents a major agricultural challenge. Thus, higher productivity must be reached through sustainable production by taking into account climate change, resources rarefaction like phosphorus and water, and losses of fertile lands. Enhancing crop diversity is increasingly recognized as a crucial lever for sustainable agro-ecological development. Growing legumes, a major biological nitrogen source, is also a powerful option to reduce synthetic nitrogen fertilizers use and associated fossil energy consumption. Organic farming, which does not allow the use of chemical, is also regarded as one prototype to enhance the sustainability of modern agriculture while decreasing environmental impacts. Here, we review the potential advantages of eco-functional intensification in organic farming by intercropping cereal and grain legume species sown and harvested together. Our review is based on a literature analysis reinforced with integration of an original dataset of 58 field experiments conducted since 2001 in contrasted pedo-climatic European conditions in order to generalize the findings and draw up common guidelines. The major points are that intercropping lead to: (i) higher and more stable grain yield than the mean sole crops (0.33 versus 0.27 kg m⁻²), (ii) higher cereal protein concentration than in sole crop (11.1 versus 9.8 %), (iii) higher and more stable gross margin than the mean sole crops (702 versus 577 € ha⁻¹) and (iv) improved use of abiotic resources according to species complementarities for light interception and use of both soil mineral nitrogen and atmospheric N₂. Intercropping is particularly suited for low-nitrogen availability systems but further mechanistic understanding is required to propose generic crop management procedures. Also, development of this practice must be achieved with the collaboration of value chain actors such as breeders to select cultivars suited to intercropping.