CuCr 2 S 4 -based solid solutions containing solute atoms on the Cu or Cr site were studied with the aim of changing the band structure of the spinel to semiconducting, while maintaining a high magnetic ordering temperature. Cu 1 -x M x Cr 2 S 4 and CuCr 2 -x M x S 4 (M = Al, Ga, In, Fe, Co, As) quaternary phases were synthesized, and CuCr 2 S 4 , Cu 0.3 Co 0.7 Cr 2 S 4 , and Cu 0.5 Fe 0.5 Cr 2 S 4 single crystals were prepared using high-temperature solution growth and chemical vapor transport. The magnetic materials were characterized by a variety of techniques.