To investigate the environmental advantages of using grass-clover binary mixtures over pure stands as winter cover crops, a serial of five field experiments (each designed as randomized complete blocks with four replicates) was carried out in eastern Slovenia. Trifolium incarnatum L. and Lolium multiflorum Lam. were sown in late summer as pure stands and binary mixtures. Pooled data calculated from all the experiments revealed that the soil mineral N in spring and accumulation of N by plants decreased with decreasing proportion of T. incarnatum in the binary mixtures, while the C:N ratio of cover crop organic matter increased. C accumulation was the highest when the seeding ratio of the binary mixture of T. incarnatum and L. multiflorum was 50:50. In the C and N environmentally sustainable management efficiency coefficients, three important traits of winter cover crops for environmental protection were given equal importance (low soil mineral N content in spring, high C accumulation in plants, and high N accumulation in plants). The coefficient was higher for binary mixtures of T. incarnatum and L. multiflorum than for pure stands of these crops, proving the complex environmental advantages of binary mixtures over pure stands.