Methods for preparation of solid solutions (hetero- and homosubstituted) in the systems InP-CdTe and CdS-CdTe have been worked out. The prepared solid solutions have been attested, on the basis of the X-ray diffraction, microscopic, electron microscopic, and optical studies results, as the substituted solid solutions with the structure of sphalerite and wurtzite, respectively; average dimensions (dav) and average numbers (nav) for the most representative particles of components and values of the band gap (Delta E) for the solid solutions have been determined. Acid-base properties of the surfaces for the systems components have been studied; their weak acidic character at relatively increased acidity of the solid solution surfaces of the InP-CdTe system has been demonstrated. Dependences of the volume and surface properties on the composition have been established. The found similarity and differences in behavior of the systems solid solutions have been explained by predominant influence of either the common component (CdTe) or the components (InP, CdS) differing in values of the band gap, difference in electronegativities difference, and ionic bonding contribution. Considerations concerning the possibilities of looking for new adsorbents-materials for semiconducting gas analysis-have been proposed.