Provided herein are methods of synthesizing large-pore periodic mesoporous quartz. Using the methods herein, large-pore periodic mesoporous quartz has been synthesized at a lower pressure and a temperature than in any previous mesoporous crystalline method, yielding a unique mesoporous article having crystalline pore walls. For example, the methods involve modified nanocasting methods using a mesoporous starting material comprising silica, carbon as a an infiltrating pore filler, followed by application of pressure and heat sufficient to crystallize silica in the infiltrated starting material to form a mesoporous crystalline article having crystalline pore walls therein, and useful in many applications, including as a catalyst.