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Sustainability of maize-based cropping systems is a major challenge for southern Africa, yet the demand for maize as staple food and animal feed in the region continues to increase. A study was conducted on a sandy clay loam (220 g clay kg^-1 soil) at Domboshawa in Zimbabwe to investigate the long-term effects of organic resource quality and application rate, and nitrogen (N) fertilization on soil chemical properties and maize (Zea mays L.) productivity. Crotalaria juncea (high quality), Calliandra calothyrsus (medium quality), cattle manure (variable quality), maize stover and Pinus patula sawdust (both low quality) were incorporated into soil at 4.0 t C ha^-1 (high rate) and 1.2 t C ha^-1 (low rate) at the start of each cropping season for nine consecutive years. At both high and low application rates, each of the five organic resources was applied in combination with or without mineral nitrogen (N) fertilizer at 120 kg N ha^-1. The nine-year period saw maize grain yields declining by 22% to 84% across treatments despite increases in soil organic carbon, total N and available P from 6% to 80%. Crotalaria, Calliandra and manure led to a less steep yield decline. Exchangeable calcium (Ca), magnesium (Mg) and potassium (K), and soil pH explained much of the variation in yield patterns observed under the different organic resource applications. Maize grain yield was positively correlated with exchangeable Ca (r = 0.51), Mg (r = 0.62) and K (r = 0.53), and soil pH (r = 0.49), but negatively correlated with other soil properties over the 9-year period. We concluded that declining soil exchangeable basic cations were the underlying causes of decreasing …