Cu2ZnSnS4 thin films with thicknesses ranging from 0.35 to 1.85 μm and micron-sized grains (0.5-1.5 μm) were synthesized using co-electrodeposited Cu-Zn-Sn-S precursors with different deposition times. Here we have introduced a sputtered CdS buffer layer for the development of CZTS solar cells for the first time, which enables breakthrough efficiencies up to 6.6%.