This study investigated the effects of delayed harvesting, varying meteorological conditions, and barley variety on Fusarium spp. infection rates, nutritional composition, and mycotoxin contamination in barley grains. Field experiments were conducted from 2020 to 2022 and involved two barley varieties: ‘Laureate’ for malting and ‘Luokė’ for feed. The results indicated that the dominant Fusarium species isolated were F. avenaceum, F. culmorum, F. poae, F. sporotrichioides, F. tricinctum, and F. equiseti. These tended to increase in number with delayed harvest times and were more prevalent during harvest periods of higher precipitation (p < 0.05). Malting barley had higher starch and lower protein content compared to feed barley (p < 0.05). Delayed harvesting generally increased dry matter, crude fat, and crude ash contents while decreasing crude protein, zinc, and iron contents (p < 0.05). Mycotoxin analysis revealed significant differences under specific weather conditions. HT-2 toxin levels were higher under slightly warmer and wetter conditions during flowering, with harvest conditions similar to the long-term average. Zearalenone levels increased with dry, warm growing seasons followed by rainy harvests. Nivalenol and enniatin levels increased with rainy growing seasons and dry, warm harvests. Deoxynivalenol concentrations did not reach the limit of quantification throughout the study. No consistent trend was observed for higher contamination in any specific barley variety (p > 0.05). The strongest correlations between mycotoxins and nutritional value indicators were observed with less-studied mycotoxins, such as nivalenol and enniatins, which exhibited negative correlations with crude protein (p < 0.01), crude fat (p < 0.05), and zinc (p < 0.01), and positive correlations with crude ash (p < 0.05) and phosphorus (p < 0.01).