The demand for gluten-free (GF) bread is steadily increasing. However, the production of GF bread with improved baking quality and enhanced nutritional properties remains a challenge. In this study, we investigated the effects of adding psyllium fibre (PSY) in varying proportions to buckwheat flour on the dough characteristics, bread quality, and starch digestion properties of GF bread. Our results demonstrate that incorporating PSY contributes to the formation of a gluten-like network structure in the dough, leading to an increase in the gas holding capacity from 83.67% to 98.50%. The addition of PSY significantly increased the specific volume of the bread from 1.17 mL/g to 3.16 mL/g. Bread containing PSY displayed superior textural characteristics and colour. Our study also revealed that the inclusion of PSY reduced the digestibility of starch in GF bread. These findings highlight the positive impact of incorporating PSY into GF bread, suggesting its potential in guiding the production of GF bread with a lower glycaemic index. This may be particularly beneficial for individuals seeking to regulate their blood sugar levels or adopt a low-glycaemic diet.