High concentrations of airborne pollen trigger seasonal allergies and possibly more severe adverse respiratory and cardiovascular health events. Predicting pollen concentration accurately is valuable for epidemiological studies, in order to study the effects of pollen exposure. We aimed to develop a spatiotemporal machine learning model predicting daily pollen concentrations at a spatial resolution of 1 × 1 km across Switzerland between 2000 and 2019. Daily pollen concentrations for five common, highly allergenic pollen types (hazel, alder, birch ash, and grasses) were available from fourteen measurement sites across Switzerland. We considered several predictors such as elevation, species distribution, wind speed, wind direction, temperature, precipitation, relative humidity, satellite-observed Normalized Difference Vegetation Index, and land-use (CORINE, Landsat satellite) to explain variation in pollen concentration. We employed feature engineering techniques to encode categorical variables and fill in missing values. We applied a random forest machine learning model with 5-fold cross-validation. The 5th–99th percentiles for concentrations of hazel, alder, birch, ash, and grass pollen at the pollen monitoring stations were 0–298, 0–306, 0–1153, 0–800, and 0–290 pollen grains/m3, respectively. The results of a predictive model for these concentrations yielded overall R2 values of 0.87, 0.84, 0.89, 0.88, and 0.91, and temporal root mean squared errors (RMSEs) of 16.07, 16.72, 69.04, 41.50, and 22.45 pollen grains/m3. An analysis of predictor variable importance indicates that the average national daily pollen concentration is the most important predictor of pollen concentrations for all pollen types. Furthermore, meteorological variables including temperature, total precipitation, humidity, boundary layer height, wind speed, and wind direction, as well as date and satellite features, are important factors in pollen concentration prediction. These spatiotemporal pollen models will serve to estimate individual residential pollen exposure for epidemiological studies. Resulting estimates will enable us to study respiratory and cardiovascular mortality and hospital admissions in Switzerland.