Allergic diseases are prevalent worldwide, and may result from exposure to various substances. Exposure to ambient bioaerosols is a potential risk factor for allergic diseases; however, accurate exposure assessment is challenging due to the limited number of outdoor monitoring stations. In this study, the relationships between ambient bioaerosol exposure and allergic diseases (i.e., acute conjunctivitis, allergic rhinitis, and asthma) were evaluated using validated land-use regression (LUR) models to estimate the exposure levels. Data on the daily outpatient visits were retrieved from the Taiwan National Health Insurance Research Database. The total fungal spore count was associated with acute conjunctivitis in males at the second and third quartiles with relative risks (RRs) of 1.75 (95% confidence interval [CI] = 1.24, 2.48) and 1.32 (95% CI = 1.03, 1.70), respectively. It was also associated with asthma in both sexes when concentration ≥ 95th percentile with RRs = 3.06 (95% CI = 1.89, 4.95) in males and 1.73 (95% CI = 1.08, 2.76) in females. Cladosporium was correlated with acute conjunctivitis in females at a concentration ≥ 95th percentile with RR = 2.90 (95% CI = 1.40, 6.04). Basidiospores were associated with allergic rhinitis in males at the third and fourth quartiles with RRs = 1.88 (95% CI = 1.44, 2.45) and 1.49 (95% CI = 1.20, 1.84), respectively. Meteorological parameters including relative humidity and rainfall were also crucial factors associated with the number of outpatient visits. Our results revealed that ambient fungal spores are crucial determinants of allergic diseases. In addition, the use of LUR models is feasible for assessing the exposure of ambient bioaerosols.