A method of synthesizing chabazite zeolites with controlled aluminum distribution. The method utilizes a source of an organic structure-directing agent, a source of an inorganic structure-directing agent, a source of aluminum and a source of silicon to form a synthesis gel which is subjected to a crystallization process to crystallize a chabazite zeolite with controlled aluminum distribution. A chabazite zeolite structure with controlled aluminum distribution. The structure contains zeolite crystal lattice framework containing silicon, aluminum, and oxygen; and extra-framework positions containing non-divalent chemical species such that each aluminum atom in the zeolite crystal lattice framework is in an isolated configuration. Another variant of this structure wherein a fraction of the aluminum atoms in the zeolite crystal lattice framework positions are not in an isolated configuration and hence oxygen atoms associated with aluminum atoms in the fraction can bind with the non-aluminum cations in the extra-framework positions.