Light absorption and carrier transfer, are two sequential and complementary steps related to photocatalysis performance, whereas the collective integration of these two aspects into graphitic carbon nitride (g-CN) photocatalyst through polycondensation optimization have seldom been achieved. Herein, we report on tailoring the crystalline structure of g-CN by avoiding the formation of incompletely reacted N-rich intermediates and selective breaking the hydrogen bonds between the layers of g-CN simultaneously. The obtained layer plane ordered porous carbon nitride (LOP-CN) material shows efficient photocatalytic H generation performance. The highest H evolution rate achieved is 53.8 μmol under λ ≥ 400 nm light irradiation, which is 7.4 times higher than that of g-CN prepared by convention thermal polycondensation. The substantially boosted photocatalytic activity is mainly ascribed to the efficient charge separation on long-range atomic order layer plane and the extended visible light harvesting ability. This work highlights the importance of crystalline structure tailoring in improving charge separation and light absorption of g-CN photocatalyst for boosting its photocatalytic H evolution activity.