NaBH4 sodalites were obtained by two new modified methods of crystallization: (1) autothermal synthesis and (2) crystallization with crossover from gel to melt flow in NaOH flux. Syntheses results were presented according to XRD, SEM and FTIR. Besides important features of both synthesis procedures product properties like crystal size and morphology were investigated. Spherical agglomerates of microcrystalline sodalite of composition Na7[AlSiO4]6BH4(H2O)2 were already observed after 4 h without any external heating by the autothermal procedure. Sodalites of the same average composition but in form of agglomerated nanoparticles are crystallized after very short times (2 h 30’) by the crossover reaction from gel to melt flow. Hydrogen release by heating was further studied for two selected samples with comparable composition from each synthesis procedure. Total hydrogen release by hydrolysis reaction with the internal cage water was found during heating of the autothermal product in synthetic air up to 550°C. In contrast hydrogen release from the nanocrystalline sample of crossover synthesis was not completed when heated under the same conditions. These differences were discussed in terms of crystal size and an earlier loss of the internal water from the nanocrystals of the crossover synthesis