Sponge-like porous carbon nitrides with large specific surface area are prepared by a green and facile synthesis method using melamine and biological reagent nucleobases (adenine, guanine, cytosine, thymidine and uracil) as precursors. The excellent biocompatibility and hydrogen bonding tendency of the nucleobase provides multiple binding sites for melamine, thus exhibiting preferable performance (5100.5 mu mol h(-1) g(-1)) than the traditional molecular as precursor. The enhanced photocatalytic performance benefits from the significantly increased specific surface area and average fluorescence lifetime as well as reduced bandgap, which leads to more exposed active sites, suppressed radiative recombination of photo-excited charge carriers, and improved light absorption. In this work, the effect of different nucleobases in increasing the catalytic activity is emphatically discussed in terms of spatial interaction forces and a matching hydrogen bonding mechanism is proposed. Photocatalytic hydrogen evolution experiments further demonstrate the enormous potential application of biomolecules in the modification of two-dimensional materials.