Exposure to environmental metals has been associated with health outcomes including respiratory health. Little is known about the impact of exposure to environmental metals on lung function among young children in general population. This study aimed to investigate the associations of exposure to metals with lung function among young children in a population-based cohort. A total of 1488 children aged 5–8 years attended a follow-up visit as part of the Longitudinal Investigation of Global Health in Taiwanese Schoolchildren (LIGHTS) cohort. We measured urinary samples of vanadium (median: 1.21 ng/mL; interquartile range (IQR): 0.73–1.98), manganese (median: 0.23 ng/mL; IQR: 0.13–0.47), arsenic (median: 40.51 ng/mL; IQR: 21.66–70.49), nickel (median: 1.09 ng/mL; IQR: 0.31–3.60), and cadmium (median: 0.26 ng/mL; IQR: 0.11–0.43) and performed lung function tests. Urinary vanadium concentrations were inversely associated with FVC (β coefficient for the highest quartile versus the other quartiles: −33.40, p = 0.001), FEV1 (β: −41.31, p < 0.001), FEV1/FVC ratio (β: −1.00, p = 0.009), PEF (β: −92.12, p = 0.004), and FEF25–75 (β: −82.85, p < 0.001), after adjusting for relevant confounders. Urinary manganese concentrations were inversely associated with FVC (β: −26.60, p = 0.007), FEV1 (β: −31.62, p = 0.001), PEF (β: −84.86, p = 0.009), and FEF25–75 (β: −69.21, p = 0.002). Stratification analyses found inverse associations of urinary vanadium and manganese concentrations with lung function parameters predominantly among children exposed to environmental tobacco smoke. We did not find significant associations of urinary arsenic, nickel, and cadmium concentrations with lung function parameters. In conclusion, this study adds new evidence showing inverse associations of vanadium and manganese exposure with lung function among young children in the general population. Children with environmental tobacco smoke exposure are particularly vulnerable to adverse impact of vanadium and manganese exposure on lung function.