Accurate and efficient measurement of leaf angle distribution (LAD) is important for characterizing canopy structures and understanding solar radiation regimes within the plant canopy. The main challenge for obtaining LAD is measuring the orientations of individual leaves rapidly and accurately in complex field conditions. In this letter, we propose an efficient and low-cost approach to estimate both leaf zenith and azimuth angles from smartphone photographs by using a structure from motion (SfM) point cloud and pyramid convolutional neural network (PCNN)-based leaf detection. This SfM-PCNN method first detects individual leaves from 2-D photographs by delineating leaf boundaries, while minimizing the influences of interior leaf textures. The segmented image with leaf annotations is then used to partition the 3-D SfM point cloud into leaf clusters, each of which is fit by a plane to calculate the leaf orientation. The method was validated with manual measurements for five plant species with different leaf sizes, leaf shapes, and leaf textures. The accuracy is satisfactory for a leaf-to-leaf comparison over a Euonymus japonicus Thunb. with R-squared values of 0.84 (RMSE = 6.27°) and 0.97 (RMSE = 12.61°) for zenith and azimuth angle estimations, respectively. The method allows researchers to efficiently acquire LADs of different plants with low cost yet high accuracy.