Cu-Sn binary particles were generated via spray pyrolysis from metal salt precursors with ethylene glycol as the co-solvent and reducing agent. The morphology, crystallinity, and elemental distribution of particles were tunable by changing the reaction temperature, residence time, and quench gas flow rate. Hollow porous particles were fabricated with a higher Sn concentration on the particle surface when the furnace set point was 500 C, while solid particles with a lower surface Sn concentration were generated when the furnace set point was 1000 C. Particles with spherical morphologies were obtained at long residence time conditions (4.5 s). Cu-Sn binary particles with irregular structures (e.g., pores on the particle surface, fragmented spherical particles, and lamellar fragments) were formed at short residence time conditions (0.92 s). A possible spray pyrolysis mechanism was proposed that incorporates chemical reaction steps and structural progression. By this mechanism, the metal salts are believed to sequentially undergo hydrolysis to metal hydroxides, decomposition to metal oxides, reduction to metals, and finally diffusion of Sn into the Cu matrix to generate the Cu-Sn solid solution.