Grain zinc (Zn) and iron (Fe) concentrations and their responses to foliar application of micronutrients in 28 Chinese wheat landraces and 63 cultivars were investigated in a two-year field experiment. The average grain Zn and Fe concentrations were 41.8 mg kg–1 (29.0?63.3 mg kg–1) and 39.7 mg kg–1 (27.9?67.0 mg kg–1), respectively. Compared with cultivars, landraces had greater grain Zn (11.0％) and Fe (4.8％) concentrations but lower harvest index (HI), grain weight per spike (GWS), grain number per spike (GNS) and thousand grain weight (TGW). Both Zn and Fe concentrations were negatively and significantly correlated with HI, GWS, and GNS, while showed a poor association with TGW, suggesting that lower HI, GWS, and GNS, but not TGW, accounted for higher Zn and Fe concentrations for landraces than for cultivars. Grain Zn concentrations of both cultivars and landraces significantly increased after foliar Zn spray and the increase was two-fold greater for landraces (12.6 mg kg–1) than for cultivars (6.4 mg kg–1). Foliar Fe spray increased grain Fe concentrations of landraces (3.4 mg kg–1) and cultivars (1.2 mg kg–1), but these increases were not statistically significant. This study showed that Chinese wheat landraces had higher grain Zn and Fe concentrations than cultivars, and greater increases occurred in grain Zn concentration than in grain Fe concentration in response to fertilization, suggesting that Chinese wheat landraces could serve as a potential genetic source for enhancing grain mineral levels in modern wheat cultivars.