Sub-Saharan African smallholder farmers face challenges due to limited access to commercial fertilizers, affecting food security. Exploring the benefits of intercropping is promising, but evaluating crop performance in specific agroecological contexts is crucial. This study in Vilankulo, Mozambique, conducted over two growth seasons (2018 and 2019), aimed to assess the benefits of intercropping maize (Zea mays L.) and cowpea (Vigna unguiculata L., Walp) (M+C) compared to maize (M) and cowpea (C) as sole crops. Key variables for comparison included dry matter yield (DMY), land equivalent ratio (LER), competitive ratio (CR), tissue nutrient concentration, nutrient recovery, and apparent N fixation (ANF). This study also examined the effects on cabbage (Brassica oleracea L.), cultivated as a succeeding crop, and soil properties. In 2018, maize plants were severely affected by drought and did not produce grain. This year, cowpea grain yields were 2.26 and 1.35 t ha−1 when grown as sole crop or intercropped. In 2019, maize grain yield was 6.75 t ha−1 when intercropped, compared to 5.52 t ha−1 as a sole crop. Cowpea grain yield was lower when intercropped (1.51 vs. 2.25 t ha−1). LER values exceeded 1 (1.91 and 1.53 for grain and straw in 2019), indicating improved performance in intercropping compared to sole crops. In 2019, CR was 1.96 for maize grain and 0.58 for cowpea grain, highlighting the higher competitiveness of maize over cowpea. Cowpea exhibited higher average leaf nitrogen (N) concentration (25.4 and 37.6 g kg−1 in 2018 and 2019, respectively) than maize (13.0 and 23.7 g kg−1), attributed to its leguminous nature with access to atmospheric N, benefiting the growth of maize in intercropping and cabbage cultivated as a succeeding crop. Cowpea also appears to have contributed to enhanced phosphorus (P) absorption, possibly due to access to sparingly soluble P forms. In 2019, ANF in M+C was 102.5 kg ha−1, over 4-fold higher than in C (25.0 g kg−1), suggesting maize accessed more N than could cowpea provide, possibly through association with endophytic diazotrophs commonly found in tropical grasses.