Barium strontium titanate ((Ba,Sr)TiO3) nanosized powders were synthesized via spray pyrolysis of a liquid precursor mist in Ar–O2 radio frequency induction thermal plasma. To adjust the cation stoichiometry of the complex oxide, liquid precursors were prepared by mixing titanium butoxide (Ti(OBu)4) stabilized with diethanolamine and aqueous solutions of barium nitrate (Ba(NO3)2) and strontium nitrate (Sr(NO3)2) stabilized with citric acid. The molar ratios of titanium, barium, and strontium ions (Ba/(Ba+Sr) and (Ba+Sr)/Ti ratios) in the liquid precursor were varied. Pure, high‐crystalline (Ba,Sr)TiO3 (Ba/(Ba+Sr)=0.0–1.0) powders of ∼45 nm in size were synthesized in this one‐step process.