The invention discloses a method for preparing Ni-BaTiO3 compound powder, which has the steps as follows: adding tetraisopropyl titanate source in a nitric acid solution to prepare a Ti source solution; adding soluble salts of Ni and Ba and reducing agent urea to prepare a precursor solution in terms of stoichiometric ratio; and spraying the solution in a vertical type reaction furnace in an ultrasonic spraying mode, and performing thermal decomposition reaction at the temperature of 750-1,000 DEG C to prepare the Ni-BaTiO3 compound powder.