In this chapter, we describe four kinds of non-stoichiometric compound, which are or will be in practical use, from the viewpoint of preparation methods or utility. As a first example, the solid electrolyte (ZrO2)0.85(CaO)0.15 is described, which are discussed in Sections 1.4.6–1.4.8 from the viewpoint of basic characteristics. The second example is the magnetic material Mn–Zn ferrite, for which the control of non-stoichiometry and the manufacturing process will be described. Then the metal hydrides or hydrogen absorbing alloys, which are one of the most promising materials for storing and transporting hydrogen in the solid state, are described, mainly focusing on the phase relation. Finally, we describe the relation between the control of composition and the growth of a single crystal of the semiconductive compound GaAs, which is expected to give electronic materials for 1C and LSI etc. Solid electrolytes, which show ionic conductivity in the solid state, are considered to be potential materials for practical use, some are already used as mentioned below. Solid electrolytes have characteristic functions, such as electromotive force, ion selective transmission, and ion omnipresence. Here we describe the practical use of calcia stabilized zirconia (CSZ), (ZrO2)0.85(CaO)0.15, the structure and basic properties of which are discussed in detail in Sections 1.4.5–1.4.8. The most simple practical application of CSZ is for the gauge of oxygen partial pressure, as mentioned in Sections 1.4.7 and 1.4.8. The oxygen partial pressure P2o2 in the closed system as shown in Fig. 3.1 can be measured, taking the air as the standard oxygen pressure P1o2. The electromotive force (EMF) of this concentration cell is expressed as . . . E = (RT/4F)ln(P1o2/ P2o2) . . . This principle is applied in the measurement of oxygen partial pressure in laboratory experiments and of the oxygen activity of slag in refineries. Based on the principle of coulometric titration (see Section 1.4.8), the oxygen partial pressure of a closed system can be kept constant by feedback of the EMF, in the oxygen pressure range 1 to 10−7 atm. By use of this closed system, investigations on redox reactions of metals and also enzyme reactions have been carried out.