Our hybrid computational / experimental approach allowed us to find new solvated structures for TMA, including the targeted hexagonal crystal packing, 1, and for ADTA, including structures with lower degrees of hydrogen bond network interpenetration that supplement the known 5-fold form. Furthermore, a desolvated porous polymorph of TMA, TMA (SA BET = 910 m 2 /g), was found by solvent exchanging one of these structures (TMA_2-33) with pentane. The crystal structure of TMA matched well with the lowest-energy predicted structure from a pronounced 'spike' in the CSP landscape. This demonstrates that this combination of computation and HT crystallization can accelerate discovery for materials with desirable physical properties, such as microporosity.