Compact storage systems demonstrating increased hydrogen storage capacity are the key to advancing the growth of the hydrogen economy throughout the world and reducing the global dependence on fossil fuels for transportation. The use of highly porous adsorbent materials for reversible hydrogen storage is a promising pathway towards achieving storage densities capable of reaching driving ranges comparable to gasoline automobiles without high-pressure compressed gas storage systems (>200 bars H₂). The focus of this effort is the enhancement of solid-state hydrogen adsorption systems through the development and inclusion of a microchannel thermal management device for efficient heat removal and uniform gas distribution in compressed beds of activated carbon and metal organic framework. The stainless steel microchannel device utilizes 250 μm walls to remove heat from the contacting adsorbent bed with liquid nitrogen coolant flow through 250 μm channel. Cryogenic (<140 K) hydrogen adsorption experiments were completed with and without liquid nitrogen cooling at pressures between 50 and 55 bars. The experiments demonstrate that the use of liquid nitrogen coolant effectively lowers the adsorbent bed temperature by removing the majority of the heat generated during the adsorption process, resulting in an 11% increase in stored H₂ gas with MOF-5 and a 3% increase with activated carbon compared to their respective non-cooled counterparts. The liquid cooled MOF-5 adsorbent bed increases average hydrogen storage throughout the experimental vessel by 14% compared to a cryo-compressed gas system at similar conditions (121 K and 55 bars). A functional development tool representing the experimental adsorption system was developed in COMSOL Multiphysics and utilized derived conservation equations and the modified Dubinin-Astakhov equation to characterization the gas flow, energy transport, and physical adsorption of supercritical hydrogen on MOF-5 adsorbent. Simulated adsorption experiments, modeled with development tool, were validated against experimental data; the predicted temperature responses at embedded thermocouple locations show a strong correlation to experimental data. The development tool may assist in the design and development of future storage systems utilizing adsorbent materials with known physical, thermal, and adsorption parameters.