In order to better understand the source-sink flow and relationships of Zinc (Zn) and other nutrients in wheat (Triticum aestivum L.) plants for biofortification and improving grain nutritional quality, effects of reducing photoassimilate source (through the flag leaf removal and spike shading) or sink (through 50% spikelets removal) in the field on accumulation of Zn and other nutrients in wheat grains of two cultivars (Jimai 22 and Jimai 44) were investigated under two soil Zn application levels. The single panicle weight (SPW), kernel number per spike (KNPS), thousand kernel weight (TKW), total grain weight (TGW), concentrations and yields of various nutrient elements (Zn, Fe, Mn, Cu, N, P, K, Ca and Mg), phytate phosphorus (phytate-P), phytic acid (PA) and phytohormones (ABA: abscisic acid, and the ethylene precursor ACC: 1-aminocylopropane-1-carboxylic acid), and C/N ratios were determined. Soil Zn application significantly increased concentrations of grain Zn, N and K. Cultivars showing higher grain yields had lower grain protein and micronutrient nutritional quality. SPW, KNPS, TKW (with an exception of TKW in half spikelets removal), TGW, and nutrient yields in wheat grains were most severely reduced by half spiklets removal, secondly by spike shading, and slightly by flag leaf removal. Grain concentrations of Zn, N and Mg consistently showed negative correlations with SPW, KNPS and TGW, but positively with TKW. There were general positive correlations among grain concentrations of Zn, Fe, Mn, Cu, N and Mg, and bioavailability of Zn and Fe (estimated by molar ratios of PA/Zn, PA × Ca/Zn, PA/Fe, or PA × Ca/Fe). Although concentrations of Zn and Fe were increased and Ca was decreased in treatments of half spikelets removal and spike shading, the simultaneously increased PA limited the increase in bioavailability of Zn and Fe. In general, different nutrient elements interact with each other and are affected to different degrees by source-sink manipulations. Elevated endogenous ABA levels and ABA/ACC ratios were associated with increased TKW and grain-filling of Zn, Mn, Ca and Mg, and inhibited K in wheat grains. However, effects of ACC were diametrically opposite. These results provide basis for wheat grain biofortification to alleviate human malnutrition.