Graphene oxide sheets have recently gained immense interest as a building block for graphene based materials and devices. Rapid developments have been made in the chemistry and applications of GO. However, assembly, too, plays a critical role in the final properties of bulk graphene based materials as it determines the microstructures of the 2D sheets. There is thus a pressing need for controllable assembly strategies. Based on the recent identification of the pH dependent surfactant-like behavior of GO sheets, we are now able to control the tiling morphologies of such sheets to produce thin films with either wrinkled or overlapped types of microstructures. This allows for the deconvolution of the effects of these two basic morphological features in the electrical and optical properties of the resulting thin films, providing a well-defined example of the processing-microstructure-properties relationship for this unique soft material building block.