The synthesis of carbon-based nanomaterials, ideally produced via facile, inexpensive approaches, using sustainable resources as precursors, with modulated structures, morphologies and functionalities is still challenging for energy applications. This work developed a mild one-step hydrothermal synthesis route for the fabrication of highly dispersed metallic nickel nanoparticles on hydrothermal carbons derived from waste biomass. The roles of precursor nickel ion concentration and calcination temperature in modulating the morphology, location and crystalline size of the nickel nanoparticles as well as the metal-support interactions have been delineated. The average grain size of the metallic nickel nanocrystals on the resultant Ni-0.5@HCOp nanocatalysts could be tuned to 8-13 nm by varying the preparation conditions. The catalytic abilities of the Ni-based nanocatalysts towards hydrogen-rich syngas production and tar reduction were then tested in a two-stage reactor system using sewage sludge as biomass feedstock. The catalytic tests showed that the Ni-0.5@HCOp catalyst calcined at 700 degrees C was shown to have stronger metal-support interactions compared to other Ni-based nanocomposites, which provided better suppression of coke deposition and resistance of nickel agglomeration during the catalytic gasification process. This highly active catalyst promoted formation of hydrogen-rich syngas, with up to 109.2 g H-2/kg sludge, and tar yields as low as 2.12 mg g(-1).