Mapping and monitoring of leaf area index (LAI) is important for spatially distributed modeling of vegetation productivity, evapotranspiration, and surface energy balance. Global LAI surfaces will be an early product of the MODIS Land Science Team, and the requirements for LAI validation at selected sites have prompted interest in accurate LAI mapping at a more local scale. While spectral vegetation indices (SVIs) derived from satellite remote sensing have been used to map LAI, vegetation type, and related optical properties, and effects of Sun–surface–sensor geometry, background reflectance, and atmospheric quality can limit the strength and generality of empirical LAI–SVI relationships. In the interest of a preliminary assessment of the variability in LAI–SVI relationships across vegetation types, we compared Landsat 5 Thematic Mapper imagery from three temperate zone sites with on-site LAI measurements. The sites differed widely in location, vegetation physiognomy (grass, shrubs, hardwood forest, and conifer forest), and topographic complexity. Comparisons were made using three different red and near-infrared-based SVIs (NDVI, SR, SAVI). Several derivations of the SVIs were examined, including those based on raw digital numbers (DN), radiance, top of the atmosphere reflectance, and atmospherically corrected reflectance. For one of the sites, which had extreme topographic complexity, additional corrections were made for Sun–surface–sensor geometry. Across all sites, a strong general relationship was preserved, with SVIs increasing up to LAI values of 3 to 5. For all but the coniferous forest site, sensitivity of the SVIs was low at LAI values above 5. In coniferous forests, the SVIs decreased at the highest LAI values because of decreasing near-infrared reflectance associated with the complex canopy in these mature to old-growth stands. The cross-site LAI–SVI relationships based on atmospherically corrected imagery were stronger than those based on DN, radiance, or top of atmosphere reflectance. Topographic corrections at the conifer site altered the SVIs in some cases but had little effect on the LAI–SVI relationships. Significant effects of vegetation properties on SVIs, which were independent of LAI, were evident. The variability between and around the best fit LAI–SVI relationships for this dataset suggests that for local accuracy in development of LAI surfaces it will be desirable to stratify by land cover classes (e.g., physiognomic type and successional stage) and to vary the SVI.