We have newly synthesized the zeolitic cobalt silicate catalysts via a simple hydrothermal treatment of borosilicate MWW precursor with Co precursor solution. As the hydrothermal temperature increased, a structural transformation occurred, shifting from three-dimensional (3D) to two-dimensional (2D) delaminated MWW layers (DML), and further to 2D amorphous phyllosilicate, accompanied by a continuous increase in Co content. The synthesized bi-functional 2D cobalt silicate facilitates the selective catalytic oxidation of NH3 (NH3-SCO), a process that requires both surface acidity and redox characteristics. In particular, Co-DML-160 prepared by hydrothermal treatment at 160 °C exhibited the coexistence of Co3O4 and framework Co species resulting in a strong redox ability and high Lewis acidity, respectively, due to their synergetic effect.