Optimisation of the concentrations of essential mineral elements in staple grain diet and reduction in non-essential and potentially toxic elements would considerably alleviate mineral malnutrition and improve the health of humans. Here, wheat (Triticum aestivum L.) plants were biofortified with Zn and/or Se to determine the changes across 36 elements in the grain. The element concentrations were determined by multielemental k 0 -instrumental neutron activation analysis (k 0 -INAA). In comparison to grain from non-biofortified plants, Zn fertilisation increased the grain Zn, Ca, and Mo concentrations, whereas the foliar application of Se only increased the grain Se concentrations. Double biofortification (combined Zn fertilisation and foliar Se) was more effective for the increased Se concentrations in the grain, in comparison to the Se-only biofortified plants, with the grain Zn, Ca and Mo concentrations remained at the same levels as those for the Zn-only biofortified plants. Except for Ba, Br and Rb, the concentrations of the elements analysed were below the detection limits. Double biofortification might be a feasible strategy to efficiently coordinate the mineral quality of wheat grain, although the considerable concentrations of other essential and non-essential elements should not be neglected.