The Festuca arundinacea Schreb. is one of the most used forage grasses due to its duration, productivity, great ecological breadth, and adaptability. Livestock has been criticized for its large production of greenhouse gases (GHG) due to forage. The advancement of science has led to an increase in the number of studies based on nanotechnologies; NPs supplementation in animal nutrition has found positive results in the fermentation of organic matter and the production of fatty acids and ruminal microorganisms. The objectives of this study were (1) to evaluate the in vitro digestibility of forage containing selenium (Se) nanoparticles (NPs), and to identify the specific behavior of the ruminal fermentation parameters of F. arundinacea Schreb. and (2) quantify the production of greenhouse gases (total gas and methane) (3) as well as the release of bioactive compounds (phenols, flavonoids, tannins, and selenium) after fermentation. Three treatments of SeNPs were established (0, 1.5, 3.0, and 4.5 ppm). The effects of foliar fertilization with SeNPs son digestion parameters were registered, such as the in vitro digestion of dry matter (IVDM); total gas production (Atotal gas) and methane production (ACH4); pH; incubation time(to); the substrate digestion rate (S); tSmax and the lag phase (L); as well as the production of volatile fatty acids (VFA), total phenols, total flavonoids, and tannins in ruminal fluid. The best results were obtained in the treatment with the foliar application of 4.5 ppm of SeNPs; IVDMD (60.46, 59.2, and 59.42%), lower total gas production (148.37, 135.22, and 141.93 mL gDM-1), and CH4 (53.42, 52.65, and 53.73 mL g DM-1), as well as a higher concentration of total VFA (31.01, 31.26, and 31.24 mmol L-1). The best results were obtained in the treatment with the foliar application of 4.5 ppm of SeNPs in the three different harvests; concerning IVDMD (60.46, 59.2, and 59.42%), lower total gas production (148.37, 135.22, and 141.93 mL gDM-1), and CH4 (53.42, 52.65, and 53.73 mL g DM-1), as well as a higher concentration of total VFA (31.01, 31.26, and 31.24 mmol L-1). The F. arundinacea Schreb plants fertilized with 4.5 ppm released—in the ruminal fluid during in vitro fermentation—the following contents: total phenols (98.77, 99.31, and 99.08 mgEAG/100 mL), flavonoids (34.96, 35.44, and 34.96 mgQE/100 g DM), tannins (27.22, 27.35, and 27.99 mgEC/100g mL), and selenium (0.0811, 0.0814, and 0.0812 ppm).