A crystalline, core-shell hybrid Chabazite (CHA) material for use as a catalyst has a core with a silicon to aluminum ratio (SAR) that is less than 25 and a shell that at least partially encapsulates the core, the shell having an SAR of about 25 or greater. The crystalline, core-shell hybrid Chabazite is prepared by forming a first chabazite (CHA) material having a silicon to aluminum ratio (SAR) that is less than 25, placing the first CHA material into an aqueous reaction mixture comprising one or more precursors capable of forming a second chabazite (CHA) material having an SAR that is 25 or greater, growing the second CHA material on the surface of the first CHA material, and collecting the core-shell hybrid CHA material.