Carbon nitride has attracted significant interest as robust, low-cost alternative to metal-based materials in fields such as photo, electro and heterogeneous catalysis. However, the properties of the final material are hard to control by traditional synthetic methods Herein, we introduce a new strategy of material design that allows controlling the desired properties of the final material already from the molecular level by sequential solvent treatment of supramolecular aggregates that serve as the reactants. Due to in situ formation of a thermodynamic driven energy levels gradient, the as-prepared carbon nitride exhibits almost 10 times higher activity than the traditional carbon nitride (calcined from melamine) in the hydrogen evolution text. As a multifunctional catalyst, the core-shell like carbon nitride also shows a superior catalytic degradation activity for RhB and p-nitrophenol. (C) 2016 Elsevier B.V. All rights reserved.