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Semiconductor heterojunction plays a pivotal role in photocatalysis. However, the construction of a heterojunction with a fine microstructure usually requires complex synthetic procedures. Herein, a pH-adjusted one-step method was employed to controllably synthesize Ag4V2O7/Ag3VO4heterojunction with a well-tuned 0D/1D hierarchical structure for the first time. It is noteworthy that the ordered stacking of vanadium oxide tetrahedron (VO3−)guided by the pH value wisely realizes the in-situgrowth of Ag4V2O7nanoparticles on the surface of Ag3VO4nanorods. Furthermore, comprehensive characterization and calculation decipher the electronic structures of Ag4V2O7and Ag3VO4and the formation of Z-scheme heterojunction, benefiting the visible light harvesting and carrier utilization. Such a new Ag4V2O7/Ag3VO4heterojunction exhibits remarkable photocatalytic activity and excellent stability. Complete degradation of Rhodamine B (RhB) can be achieved in 10 min by the Ag4V2O7/Ag3VO4heterojunction under visible light irradiation, demonstrating an outstanding reaction rate of 0.35 min−1that is up to 84-fold higher than those of other silver vanadates. More importantly, this integration of synthesis technology and heterojunction design, based on the intrinsic crystal and electronic structures, could be inspiring for developing novel heterostructured materials with advanced performance.