Diverse methods have been developed for the synthesis of active nanocatalysts involving various heterogeneous catalytic reactions. Thus far, numerous trial-and-error runs have been done to find the effective and practical ways. In the present work, the All-In-One (AIO) reactor system with a well-designed synthesis program, now in pilot stage, was first exploited as a reliable synthesis tool to find the optimum conditions for the production of Ni nanocatalysts. Using an activated charcoal support, active Ni nanoparticles of 7.8.11.8 nm (labeled A001-A007 in the program) were produced. These were achieved using a melt-impregnation process, which was controlled by variations in the applied gas (N2 and H2) and temperature (400 °C, 450 °C, and 500 °C) used as critical factors in the calcination step. Based on the optimization of the reaction sequence, each Ni nanocatalyst could be prepared within 5 h and 22 min. In particular, the optimum Ni nanocatalyst (A006) with the smallest particle size (7.8 nm), prepared under H2 flow at 400 °C, exhibits the highest catalytic activity (0.748 mmol4-NP·gcat -1·s-1) among the Ni catalysts for 4-nitrophenol (4-NP) reduction to 4-aminophenol (4-AP). This activity is much higher than that of conventional supported Ni nanocatalysts (0.551 mmol4-NP·gcat -1·s-1) produced using the wetness method.