Small-scale variations in radiative transfer through forest canopies are strongly linked to canopy structural heterogeneity. To date, upscaling of radiative transfer parameterizations developed at the point scale is hampered by (i) poor representation of canopy structure variability and (ii) limited spatially explicit subcanopy irradiance data to assess the performance of radiative transfer schemes at typical resolutions of land surface models. This study presents a novel approach for efficient in situ characterization of canopy structure and subcanopy irradiance over large spatial extents. The method involves a handheld radiometer assembly mounted on a motorized gimbal developed for nonstationary continuous measurements of shortwave and longwave radiation along forest transects. In combination with radiation and temperature data from a stationary reference station, spatially resolved estimates of sky-view fraction, canopy transmissivity, and longwave enhancement could be obtained. Under favorable meteorological conditions, validation against sky-view fraction data from hemispherical photographs yielded an RMSE of 0.03 (i.e., 3%). Irradiance measurements under heterogeneous canopy cover revealed strong spatial coherence between longwave radiation enhancement, shortwave radiation attenuation, and sky-view fraction on overcast days. Under clear-sky conditions, however, sun flecks caused highly variable shortwave radiation transmissivity patterns. This study demonstrates the potential of handheld radiometer surveys to deliver valuable spatially distributed datasets of collocated canopy structure and subcanopy irradiance which can be used (i) as reference data for alternative approaches to derive canopy structure parameters, (ii) to improve modeling of subcanopy radiation across a wide range of canopy distributions, and (iii) to support respective model upscaling efforts.