In this work, we prepared spherical gallate-based phosphors using an aerosol pyrolysis method. The synthetic parameters such as post heat-treatment temperature, activator concentration, and degree of reductions were optimized for the maximum cathodoluminescent (CL) intensity. For enhancing the CL luminous efficiency of phosphors, adjustment of lattice structure were also considered. It was found that the CL intensity was sensitive to the crystal structure in host lattice, which would be engineered by Al concentration in ZnGa-Al-O system. The most prominent result on the zinc aluminogallates which are of spherical shape was the brightness of 550 cd/m(2) at 400 V excitation with color coordinate of x = 0.1665 and y = 0.6655.