Porous carbons are extensively applied in gas separation, water purification, catalytic reaction, and electrochemical processing, attributing to their high specific surface area, large pore volume, chemical inertness, and good mechanical and thermal stability. The templating method is widely used to synthesize porous carbons with the controlled pore structure. Among them, preparation of diatomite-templated carbons attracts increasing attention because the obtained carbon has unique developed macropores and exhibits the promising application in adsorption and support of large-sized molecules. Macroporous diatomite-templated carbons are prepared by using additive or inherent solid acid sites of diatomite as the catalyst. The obtained carbons showed tubular and pillared macroporous structures, and had a few mesopores and micropores. However, the carbons possessed the small specific surface area and micropore volume, and thus showed the low adsorption capacity of small-sized molecules, such as methylene blue (MB). In this case, enhancement of porosity, especially microporosity, is necessary. Porous carbons are extensively applied in gas separation, water purification, catalytic reactions, and electrochemical processing, attributing to their high specific surface area, large pore volume, chemical inertness, and good mechanical and thermal stability. The templating method is widely used to synthesize porous carbons with the controlled pore structure. Among them, preparation of diatomite-templated carbons attracts increasing attention because the obtained carbon has unique developed macropores and exhibits the promising application in adsorption and support of large-sized molecules. Macroporous diatomite-templated carbons are prepared by using additive or inherent solid acid sites of diatomite as the catalyst. However, the carbons possessed the small specific surface area and micropore volume, and thus showed the low adsorption capacity of small-sized molecules, suc h as methylene blue (MB). In this case, enhancement of porosity, especially microporosity, is necessary.