Effects of composition and preparation method of MnNaW/SiO2 and LaSr/CaO catalysts on their physical-chemical properties and performance in oxidative coupling of methane (OCM) have been studied. For MnNaW/SiO2 catalysts the synthesis method and type of SiO2 have a significant effect on the texture, while the Na/W ratio determines the phase composition. The variation of preparation method and temperature of catalyst calcination allows regulation of the metal surface concentration and mode of metal distribution across the SiO2 support. For LaSr/CaO catalysts the synthesis method determines the specific surface area, surface and phase composition. Correlations between catalyst performance, preparation method and state of the catalyst were established. The rational preparation procedure and perspective composition of OCM catalyst have been developed. The 20La/CaO catalysts prepared by citrate sol-gel method were shown to provide ~20% C2 yield and ~40% methane conversion at 800 ºC.