This text was developed from a course for physical chemistry and chemical physics students using cross-polarization (CP) magic angle spinning (MAS) NMR in their laboratory assignments. The book provides students with the details of the CP/MAS experiment as it is used to obtain rare-spin, high-resolution NMR spectra. The design of the CP/MAS experiments and the interpretation of spectra and relaxation measurements require an understanding of the interplay of several fundamental physical interactions not normally encountered in solution NMR. The student can observe the way interacting spin systems behave in the solid state, and have a quantum mechanically rigorous understanding of solid-state spin phenomena. The text will have the added benefit of serving as a self-study resource for students seeking to learn the underlying principles of laboratory experiments using the technique. The history of NMR is also treated, and the instrumentation of the spectrometer and probe are discussed.