We report a study on the wetting and spreading of hydrazine-CZTS solution on a series of solid surfaces. The work of adhesion between a hydrazine solution and soda-lime glass, Si, graphite, ITO, SnO2, ZnO, CdS, In2S3, Cu, Au, Ag, Al, Ni, Mo, and carbon single-walled nanotubes was calculated using observed contact angles and the areas of the interface. The surface roughness of drop-casted CZTS precursor films was lower on surfaces with better hydrazine wettability. This suggests that the surface roughness of solution-processed films can be controlled by altering the wetting behavior of the solution on the substrate.