As an emerging molecular imaging modality, cone-beam X-ray luminescence computed tomography (CB-XLCT) uses X-ray-excitable probes to produce near-infrared (NIR) luminescence and then reconstructs three-dimensional (3D) distribution of the probes from surface measurements. A proper photon-transportation model is critical to accuracy of XLCT. Here, we presented a systematic comparison between the common-used Monte Carlo model and simplified spherical harmonics (SPN). The performance of the two methods was evaluated over several main spectrums using a known XLCT material. We designed both a global measurement based on the cosine similarity and a locally-averaged relative error, to quantitatively assess these methods. The results show that the SP3 could reach a good balance between the modeling accuracy and computational e±ciency for all of the tested emission spectrums. Besides, the SP1 (which is equivalent to the diffusion equation (DE)) can be a reasonable alternative model for emission wavelength over 692 nm. In vivo experiment further demonstrates the reconstruction performance of the SP3 and DE. This study would provide a valuable guidance for modeling the photon-transportation in CB-XLCT.