AbstractThe preparation of the porous graphene materials with controllable porosity basically depends on the design of porous architectures. The development of three‐dimensional (3D) graphene materials from two‐dimensional (2D) graphene sheets can harness the unique physical and electrical properties of graphene, but the challenges lie on the design and synthesis of nanoporous graphene with controlled engineering. In this work, two organic aromatic molecules viz., 2‐amino‐3‐hydroxypyridine and phloroglucinol were targeted for the development of porous graphene nanostructures. The synthesis process was designed in such a way that both the molecules having ─OH and ─NH2 groups at ortho position and 3 ─OH groups at 1, 3, 5 positions, respectively, can generate pores along with the development of graphenic lattice during heat treatment. The optimization of reaction conditions viz., time and temperature was done and the chemistry of formation of porous natured graphenic lattice was discussed. Interestingly, the results indicate that both the organic molecules have the potential to develop porous graphenic structures within their lattice at relatively low temperatures without using any additional reagents and reaction conditions. It is suggested that the structure of organic precursor is a critical factor which needs to be optimized to produce porous graphenes.