Solar-induced chlorophyll fluorescence (SIF) has been used as an indicator for the photosynthetic activity of vegetation at regional and global scales. Canopy structure affects the radiative transfer process of SIF within canopy and causes the angular-dependencies of SIF. A common solution for interpreting these effects is the use of physically-based radiative transfer models. As a first step, a comprehensive evaluation of the three-dimensional (3D) radiative transfers is needed using ground truth biological and hyperspectral remote sensing measurements. Due to the complexity of forest modeling, few studies have systematically investigated the effect of canopy structural factors and sun-target-viewing geometry on SIF. In this study, we evaluated the capability of the Fluorescence model with the Weighted Photon Spread method (FluorWPS) to simulate at-sensor radiance and SIF at the top of canopy, and identified the influence of the canopy structural factors and sun-target-viewing geometry on the magnitude and directional response of SIF in deciduous forests. To evaluate the model, a 3D forest scene was first constructed from Goddard’s LiDAR Hyperspectral and Thermal (G-LiHT) LiDAR data. The reliability of the reconstructed scene was confirmed by comparing the calculated leaf area index with the measured ones from the scene, which resulted in a relative error of 3.5%. Then, the performance of FluorWPS was evaluated by comparing the simulated at-sensor radiance spectra with the spectra measured from the DUAL and FLUO spectrometer of HyPlant. The radiance spectra simulated by FluorWPS agreed well with the measured spectra by the two high-performance imaging spectrometers, with a coefficient of determination (R2) of 0.998 and 0.926, respectively. SIF simulated by the FluorWPS model agreed well with the values of the DART model. Furthermore, a sensitivity analysis was conducted to assess the effect of the canopy structural parameters and sun-target-viewing geometry on SIF. The maximum difference of the total SIF can be as large as 45% and 47% at the wavelengths of 685 nm and 740 nm for different foliage area volume densities (FAVDs), and 48% and 46% for fractional vegetation covers (FVCs), respectively. Leaf angle distribution has a markedly influence on the magnitude of SIF, with a ratio of emission part to SIF range from 0.48 to 0.72. SIF from the grass layer under the tree contributed 10%+ more to the top of canopy SIF even for a dense forest canopy (FAVD = 3.5 m−1, FVC = 76%). The red SIF at the wavelength of 685 nm had a similar shape to the far-red SIF at a wavelength of 740 nm but with higher variability in varying illumination conditions. The integration of the FluorWPS model and LiDAR modeling can greatly improve the interpretation of SIF at different scales and angular configurations.