Using an organic solvent-based formulation, flexible and homogeneous ZrB2 tapes were cast for potential use as advanced aerospace exploration vehicles. Dispersant concentrations were optimized for attrition-milled ZrB2 powder using gravitational sedimentation and viscosity measurements. Tape cast slurry formulations with varying amounts of binder (6-8 vol%), plasticizer (7-11 vol%), and solids loading (20-23 vol%) were used to optimize the casting slurry. An optimal slurry formulation was determined based on cast tape uniform particle distribution and flexibility without cracking. Thermal gravimetric analysis of the optimized tape was used to create a binder burnout schedule that did not alter the tape structure or particle distribution. Our organic solvent-based tape casting approach results in minimum oxygen contamination after colloidal processing and robust cast tapes with a thickness of 280 mu m and green density of similar to 41% theoretic density after binder burnout.