Selenium (Se) is an essential micronutrient for human health, and enriching wheat grain with Se can improve its nutritional value. To explore practical applications, field trials tested different Se fertilisation methods and timings, aiming to increase grain Se content without compromising yield or bread-making quality. Results showed that Se fertilisation did not affect grain yield but significantly increased Se concentration in the grain. The most effective strategy combined seed treatment, soil application, and foliar sprays at the tillering and stem elongation stages—maximising Se uptake. In terms of bread-quality traits, Se had a positive effect on protein content and falling number, both key indicators for baking. All treated grain met bread-quality standards. Selenium fertilisation can therefore be considered a safe and effective way to enhance both the nutritional and technological quality of spring wheat grain. However, the timing and method of application are critical to achieving optimal results.