Based on Schiff base chemistry, crosslinked porous organic aminal networks were prepared using acetic acid as a catalyst. These Schiff base networks (SNWs) are polymeric materials based on melamine and 5,5′-methylene-bis-salicylaldehyde, with nitrogen contents as high as ca. 36 wt.%, which were characterized by FTIR spectroscopy, elemental analysis, and 13C and 15 N solid-state NMR spectroscopies. A series of polymer networks with different monomeric molar ratios and different amounts of added catalyst were explored, in order to study their effect on the final polymer structure, porosity and H2 storage capacity. These materials exhibit Brunauer-Emmett-Teller (BET) surface areas up to ca. 526 m2/g, as measured by N2 adsorption at 77 K, and exhibit gravimetric storage capacities up to 2.57 wt.% at 20 bar and 77 K.