Modeling the single-scattering properties of nonspherical particles in the atmo¬sphere (in particular, ice crystals and dust aerosols) has important applications to climate and remote sensing studies. The first part of the dissertation (Chapters II¬V) reports a combination of exact numerical methods, including the finite-difference time-domain (FDTD), the discrete-dipole-approximation (DDA), and the T-matrix methods, and an approximate method-the physical-geometric optics hybrid (PGOH) method-in the computation of the optical properties of the non-spherical particles in a complete range of size parameters. The major advancements are made on the modeling capabilities of the PGOH method, and the knowledge of the electromag¬netic tunneling effect – a semi-classical scattering effect. This research is important to obtain reliable optical properties of nonspherical particles in a complete range of size parameters with satisfactory accuracy and computational efficiency. The second part (Chapters VI-VII) of the dissertation is to investigate the de¬pendence of the optical properties of ice crystals and mineral dust aerosols in the atmosphere on the spectrum, the particle size and the morphology based on compu¬tational models. Ice crystals in the atmosphere can be classified to be simple regular faceted particles (such as hexagon columns, plates, etc.) and imperfect ice crystals. Modeling of the scattering by regular ice crystals is straightforward, as their morphologies can be easily defined. For imperfect ice crystals, the morphology is quite diverse, which complicates the modeling process. We present an effective approach of using irregular faceted particle to characterize the imperfectness of ice crystals. As an example of application, less-than-unity backscattering color ratio of cirrus clouds is demonstrated and explained theoretically, which provides guidance in the calibra¬tion algorithm for 1.064-µm channel on the Calipso lidar. Dust aerosols have no particular morphology. To develop an approach to modeling the optical properties of realistic dust particles, the principle of using simple shapes (triaxial ellipsoids and nonsymmetric hexahedra) to represent irregular dust particles is explored. Simulated results have been compared with those measured in laboratory for several realistic aerosol samples. Agreement between simulated results and measurement suggests the potential applicability of the two aforementioned aerosol models. We also show the potential impact of the present study to passive and active atmospheric remote sensing and future research works.