The current study was developed to evaluate agronomic efficiency and food security of isolated or simultaneous use of two residues-steel slag and fresh or composted poultry litter-in the cultivation of broccoli (Brassica oleracea var. italica). The composition and contribution of toxic and potentially toxic metals by different treatments and contents, translocation, and accumulation of Pb, Cd, Cu, Fe, Mn, and Zn in different plant organs were analyzed. Then, risks to human health associated with consumption of inflorescences were based on the indices of estimated daily intake, noncarcinogenic target hazard quotient, total hazard index (THI), and carcinogenic risk factor (CR), considering adults and children. Steel slag was similar to limestone in terms of the corrective effect of acidity and, despite containing toxic metals, it did not contribute to their higher translocation to inflorescences. Composting favored the concentrations of Pb, Cu, and Zn in poultry litter. The combined use of steel slag and fresh poultry litter and, mainly, composted poultry litter, favored absorption and translocation of Pb for inflorescences, that is, 60.37% and 66.13% of all Pb absorbed, respectively. Consumption of inflorescences from these treatments resulted in the critical THI values of 1.03 and 1.52, respectively, with Pb and Cd being the metals that mostly contributed to the risk. The registered CR was higher than the threshold level of 10-6. The use of steel slag associated with poultry litter favors contamination of broccoli inflorescences and increases risks to human health due to their consumption.