An advanced ammonia borane (AB)-based H2 power-pack is designed to continually drive an unmanned aerial vehicle (UAV) for 57 min using a 200-We polymer electrolyte membrane fuel cell (PEMFC). In a flight test with the UAV platform integrated with the developed power-pack, pure hydrogen with an average flow rate of 3.8 L(H2) min−1 is generated by autothermal H2-release from AB with tetraethylene glycol dimethylether (T4EGDE) as a promoter. During take-off, a hybridized power management system (PMS) consisting of the fuel cell and an auxiliary lithium-ion battery supplies 500 We at full power simultaneously, while the fuel cell alone provides 150–200 We and further recharges the auxiliary battery upon cruising. Gaseous byproducts identified by in situ Fourier transform infrared (FT-IR) spectroscopy during AB dehydrogenation are sequestrated using a mixed absorbent in an H2 purification system. In addition, a real-time monitoring system is employed to determine the remaining filter capacity of the purifier at a ground control system for rapidly responding unpredictable circumstances during flight. Separate experiments are conducted to screen potential materials and methods for enhancing filter capacity in the current H2 refining system. A prospective reactor concept for long-term fuel cell applications is proposed based on the results.