A simple chemical co-precipitation/calcination route was developed for the synthesis of simulated synroc-B and synroc-C powders using mostly nitrate salts as starting chemicals and 20% ammonia solution as precipitant. In this route, a mixed solution containing Al-nitrate, Ca-nitrate, Ba-nitrate, zirconyl nitrate and titanyl nitrate in the molar proportion required for synroc-B is added to dilute ammonia solution to precipitate these cations in the form of their hydroxides at room temperature by maintaining pH » 10.5 during precipitation. Formation of a major fluorite phase with minor amounts of anatase, rutile and hollandite phases is observed in the powder obtained after calcination in air at 750 °C. Multiphase crystalline synroc-B matrix containing hollandite, perovskite, zirconolite, and rutile phases is obtained after sintering the heat treated powder in the form of pellets at 1230 °C for 4 h in air. Similarly, pure synroc-C phases with 14 and 20% simulated waste loadings were synthesized following the same synthesis protocol. These pre-treated powders with a high surface area of ~25 m² g^-1 gave sintered ceramics having density of ~90% for 14 and 20% waste loadings.