Hydrothermal, solvothermal or ionothermal routes are usually employed for the synthesis of zeolite, which is often accompanied by a high energy consumption, high cost and low efficiency. We have developed a novel route for the rapid and high yield synthesis of mordenite (MOR) zeolite via an ice-templating method. In comparison with traditional hydrothermal synthesis, not only the high yield, but also the superior crystallinity, large reduction in water level and reaction pressure, simple device and conventional silica sources by this route can have great potential for the commercial production of pure MOR zeolite. Moreover, the changed bonding environment of silicon atoms in MOR zeolite, that is, a relative decrease in the tetrahedrally coordinated Si–O–Si bond, and accordingly, an increase in the T–OH (T = Si, Al) groups and Si–O–Al sites, remarkably enhances its acid strength.