Solution processing provides a versatile and inexpensive means to prepare functional materials with specifically designed properties. The current challenge is to mimic the structural, optical, and/or chemical properties of thin films fabricated by vacuum-based techniques using solution-based approaches. In this work we focus on ZnO to show that thin films grown using a simple, aqueous-based, chemical bath deposition (CBD) method can mimic the properties of sputtered coatings, provided that the kinetic and thermodynamic reaction parameters are carefully tuned. The role of these parameters toward growing highly oriented and dense ZnO thin films is fully elucidated through detailed microscopic and spectroscopic investigations. The prepared samples exhibit bulk-like optical properties, are intrinsic in their electronic characteristics, and possess negligible organic contaminants, especially when compared to ZnO layers deposited by sol-gel or from nanocrystal inks. The efficacy of our CBD-grown ZnO thin films is demonstrated through the effective replacement of sputtered ZnO buffer layers within high efficiency solution processed Cu2ZnSnS4xSe4(1-x) solar cells.