Abstract: Nuclear magnetic resonance (NMR) studies of small molecules dissolved in liquid crystalline solutions are presented. The works included in the dissertation are categorized into two parts: (1) variable angle spinning (VAS) and switched angle spinning (SAS) experiments for small organic molecules; (2) high-resolution NMR studies of solvent-solute interactions based on the residual dipolar coupling measurements. The dissertation is organized into four chapters. The first chapter is intended to be a brief introduction of NMR basics, focusing on what is most relevant to the experiments presented here. The second chapter introduces backgrounds of liquid crystals, and in particular, NMR spectroscopy in liquid crystals and the use of dipolar couplings for the determination of molecular structures. The third chapter explains the director reorientation methods for scaling of dipolar couplings, and simplification and information tailoring of NMR spectra of flourinated organic molecules trifluoroiodoethene and chloropentafluorobenzene in liquid crystalline solutions by VAS and SAS methodology. The fourth chapter describes NMR spectroscopy of small molecules iodomethane, bromomethane, benzene, furan, and thiophene, focusing on their different behavior in thermotropic and lyotropic liquid crystalline solutions.