The freezing of concentrated colloidal suspensions is a complex physical process involving a large number of parameters. These parameters provide unique tools to manipulate the architecture of freeze-cast materials at multiple length scales in a single processing step. However, we are still far from developing predictive models to describe the growth of ice crystals in concentrated particle slurries. In order to exert reliable control over the microstructural formation of freeze-cast materials, it is necessary to reach a deeper understanding of the basic relationships between the experimental conditions and the microstructure of the growing solid. In this work, we explore the role of several processing variables (e.g., composition of the suspension, freezing rate, and patterning of the freezing surface) that could affect the formulation strategies for the architectural manipulation of freeze-cast materials. We also demonstrate, using freeze-cast lamellar structures, that reducing the lamellar thickness by less than half increases the compressive strength by more than one order of magnitude.