This chapter is devoted to magnetic resonance spectroscopy for the investigation of unpaired electron spins. Two terms are used in the literature: electron paramagnetic resonance (EPR) and electron spin resonance (ESR). We will use the first term in this chapter. During the sixty years since its discovery in 1944 by E.K. Zavoisky [1], EPR spectroscopy has been exploited as a very sensitive and informative technique for the investigation of different kinds of paramagnetic species in solid or liquid states.The first two parts of the chapter introduce the theoretical background and instrumentation used in two complementary approaches to EPR spectroscopy, i.e., continuous-wave and pulsed EPR. The final part describes typical areas of solid state applications. spectroscopy. Space limitations preclude references to all original publications and the reader is therefore referred to earlier reviews for a more complete survey of earlier work. Excellent textbooks in EPR spectroscopy cover basic materials [2-5]. Many monographs are devoted to the consideration of more specific topics including theory, instrumentation, or application to selected paramagnetic species [6][7][8][9][10][11][12][13][14][15][16][17][18][19]. Handbooks of EPR spectroscopy [20,21] are also available, as are periodic reviews on theory, experimental approaches, and different EPR applications covering the period since 1971 [22].A comprehensive description of pulsed EPR spectroscopy is given in the recently published book of Schweiger and Jeschke [23]. Previous literature on pulsed EPR includes two monographs [24,25], several edited books [18, 19,26,27], and a large number of reviews. An up-to-date list is provided in [23]. This chapter is based on an extensive literature devoted to EPR 3. Electron Paramagnetic Resonance Spectroscopy