Hydrogen storage may be the bottle neck in hydrogen economy, where hydrogen spillover is in dispute as an effective mechanism. In this context, activated carbon (AC) was doped with nitrogen by using ammonia gas, and was further decorated with platinum, palladium, nickel, rhodium, iridium and ruthenium, via an ultrasound-assisted impregnation method, with average particle sizes of around 74, 60, 78, 61, 67 and 38 nm, respectively. The hydrogen storage was compared, before and after modification at both ambient and cryogenic temperatures, for exploring the spillover effect, induced by the decorating transition metals. Ammonia treatment improved hydrogen storage at both 298 K and 77 K, for the samples, where this enhancement was more remarkable at 298 K. Nevertheless, metal decoration reduced the hydrogen uptake of AC for all of the decorated samples other than palladium at cryogenic temperature, but improved it remarkably, especially for iridium and palladium, at room temperature. This observation suggested that metal decoration’s counter effect overcomes hydrogen spillover at cryogenic temperatures, while the opposite takes place at ambient temperature.