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Maize (Zea mays L.) is the main staple cereal food crop cultivated in southern Africa. Interactions between grain yield and biochemical traits can be useful to plant breeders in making informed decisions on the traits to be considered in breeding programs for high grain yield and enhanced quality. The objectives of this study were to estimate the heritability of grain yield and its related traits, as well as quality traits, and determine the association between quality protein maize (QPM) with non-QPM crosses. Grain yield, and agronomic and quality trait data were obtained from 13 field trials in two countries, for two consecutive seasons. Significant genotypic and phenotypic correlations were recorded for grain yield with protein content (rG = 0.38; rP = 0.25), and tryptophan with oil content (rG = 0.58; rP = 0.25), and negative rG and rP correlations were found for protein with tryptophan content and grain yield with tryptophan content. Path analysis identified ear aspect, ears per plant, and starch as the major traits contributing to grain yield. It is recommended that ear aspect should be considered a key secondary trait in breeding for QPM hybrids. The negative association between grain yield and tryptophan, and between protein and tryptophan, will make it difficult to develop hybrids with high grain yield and high tryptophan content. Hence, it is recommended that gene pyramiding should be considered for these traits.