The co-condensation of dicyandiamide and aminobenzonitrile (ABN) followed by post-calcination in NaCl-KCl molten salt can endow the Polymeric Carbon Nitride (PCN) with enhanced electron delocalization and defects (-C[tbnd]N and nitrogen defects), leading to extended optical absorption range and improved separation rate of photogenerated carriers. As a consequence, the active-optimized DCN-NaK-90ABN accounts for 76 times promotion than DCN in photodegradation of bisphenol A (BPA) under visible light. More importantly, the photocatalytic activity is demonstrated by the significantly enhanced degradation of BPA and H production under λ > 500 nm, which are much better than those of most previously reported PCN-based photocatalysts. Furthermore, the theoretical calculations certify the validity of proposed structure and explain the reactive mechanism combing with the experimental results. Our findings shed light on a new pathway for designing the efficient photocatalysts to capture the long wavelength solar power.