We exhibit the reasonable design and architect of MoS 2 @g-C 3 N 4 /g-C 3 N 4 hierarchical hetero-homojunction structure by ultrasonically pulverize and vibrate MoS 2 nanoparticles into the ultrasonically exfoliated hierarchical g-C 3 N 4 /g-C 3 N 4 homojunction slit for efficient organic pollutant photodegradation, where the g-C 3 N 4 /g-C 3 N 4 homojunction is fabricated using recrystallized urea and recrystallized dicyandiamide as double-source precursor for better photogenerated charges separation and transfer. Oil bath thermal-treatment enhances the interaction between MoS 2 nanoparticles and g-C 3 N 4 /g-C 3 N 4 nanosheets. The distinctive design accelerates the separation and transfer of photogenerated carriers, provide larger specific surface area and more active sites for organic pollutant degradation. In the composite catalyst, MoS 2 serves as the electron convergence center. Profiting from the hetero-homojunction structural merits, the optimized UOMSHCN-25 displays excellent photocatalysis activity and high stability for organic pollutant degradation (MO (96.3% within 40 min), Rh B (98.7% within 10 min) and TC (83.9% within 60 min)). Finally, a reasonable photocatalysis mechanism is proposed and discussed in detailed.