We have successfully synthesized Sr(2)V(1-x)Mo(x)O(4) from x = 0.3 to 1.0 by an improved process. The layered compound Sr(2)VO(4) is an antiferromagnetic insulator with S = 1/2, while the isostructural Sr(2)MoO(4) is a Pauli paramagnetic metal. The solid solution Sr(2)V(1-x)Mo(x)O(4) of these materials is expected to show a metal-insulator transition. In this paper we report the synthetic process and the results of the magnetic susceptibility and the electrical resistivity. The selection of the starting materials and the adjustment of O(2) partial pressure of less than 10(-12) atm were indispensable for the synthesis. The reducing conditions during the sintering had been determined rationally, according to thermodynamical analysis. Kondo-like behavior in both resistivity and magnetic susceptibility were observed in a limited range of V-containing samples.