Selenium (Se) is an essential trace element that plays a crucial role in maintaining the health of humans, animals, and certain plants. It is extensively present throughout the Earth's crust and is absorbed by crops in the form of selenates and selenite, eventually entering the food chain. Se biofortification is an agricultural process that employs agronomic and genetic strategies. Its goal is to enhance the mechanisms of crop uptake and the accumulation of exogenous Se, resulting in the production of crops enriched with Se. This process ultimately contributes to promoting human health. Agronomic strategies in Se biofortification aim to enhance the availability of exogenous Se in crops. Concurrently, genetic strategies focus on improving a crop's capacity to uptake, transport, and accumulate Se. Early research primarily concentrated on optimizing Se biofortification methods, improving Se fertilizer efficiency, and enhancing Se content in crops. In recent years, there has been a growing realization that Se can effectively enhance crop growth and increase crop yield, thereby contributing to alleviating food shortages. Additionally, Se has been found to promote the accumulation of macro-nutrients, antioxidants, and beneficial mineral elements in crops. The supplementation of Se biofortified foods is gradually emerging as an effective approach for promoting human dietary health and alleviating hidden hunger. Therefore, in this paper, we provide a comprehensive summary of the Se biofortification conducted over the past decade, mainly focusing on Se accumulation in crops and its impact on crop quality. We discuss various Se biofortification strategies, with an emphasis on the impact of Se fertilizer strategies on crop Se accumulation and their underlying mechanisms. Furthermore, we highlight Se's role in enhancing crop quality and offer perspective on Se biofortification in crop improvement, guiding future mechanistic explorations and applications of Se biofortification.