This study compared aspatial and spatial methods of using remote sensing and field data to predict maximum growing season leaf area index (LAI) maps in a boreal forest in Manitoba, Canada. The methods tested were orthogonal regression analysis (reduced major axis, RMA) and two geostatistical techniques: kriging with an external drift (KED) and sequential Gaussian conditional simulation (SGCS). Deterministic methods such as RMA and KED provide a single predicted map with either aspatial (e.g., standard error, in regression techniques) or limited spatial (e.g., KED variance) assessments of errors, respectively. In contrast, SGCS takes a probabilistic approach, where simulated values are conditional on the sample values and preserve the sample statistics. In this application, canonical indices were used to maximize the ability of Landsat ETM+ spectral data to account for LAI variability measured in the field through a spatially nested sampling design. As expected based on theory, SGCS did the best job preserving the distribution of measured LAI values. In terms of spatial pattern, SGCS preserved the anisotropy observed in semivariograms of measured LAI, while KED reduced anisotropy and lowered global variance (i.e., lower sill), also consistent with theory. The conditional variance of multiple SGCS realizations provided a useful visual and quantitative measure of spatial uncertainty. For applications requiring spatial prediction methods, we concluded KED is more useful if local accuracy is important, but SGCS is better for indicating global pattern. Predicting LAI from satellite data using geostatistical methods requires a distribution and density of primary, reference LAI measurements that are impractical to obtain. For regional NPP modeling with coarse resolution inputs, the aspatial RMA regression method is the most practical option.