In this study, submicrometer grain-sized metal matrix composites (MMCs) based on nickel were elaborated via a bottom-up strategy combining the polyol process and a non-conventional heat treatment route. First, four sets of nano-sized NiP metastable alloy nanopowders with an average particle size centered at 50, 100, 130, and 220 nm were prepared by the polyol process modified by the addition of hypophosphite (strong reducing agent) and heterogeneous nucleation using silver nitrate and platinum salt (nucleating agents). The heat treatment step was realized by reactive spark plasma sintering (R-SPS) at identical heat treatment conditions (600 • C, 53 MPa, and 10 min as holding time). R-SPS transformed the NiP metastable alloys into bulk submicrometer grain-sized MMCs with Ni as the matrix and Ni 3 P as the reinforcement. Mechanical and magnetic properties of the four MMC samples were found to be closely related to the grain size of the Ni matrix, which varied from 247 to 638 nm. Yield stress, maximum stress, and coercive field increased when the grain size decreased, while plastic strain and magnetization saturation decreased. The reinforcement Ni 3 P phase enhanced the mechanical characteristics of the composite. Crossover behavior was observed at around 350 nm Ni grain size, where a ductile and soft magnetic composite was tuned into a hard mechanical and semi-hard magnetic one.