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By using the photo-deposition technique, the Ag was selectively reduced to Ag particles that were subsequently deposited on the BiVO+4(010) facet. Subsequently, the electropositive g-C3N4 was deposited on the BiVO4(010) facet. The band bending of the interface brought on by the polarization charge and the integrated electric field worked in concert to create the BiVO4(010)–Ag–g-C3N4 crystalline plane S-type heterojunction. As a result, carriers live longer, e−–h pair recombination is successfully prevented, and the heterojunction’s redox capability has enhanced. After 150 min irradiation under Vis/NIR light, the degradation rate of 20 mg/L TC by crystalline S-type heterojunctions reaches 78.79%/53.70%, respectively, and the degradation rates of heterojunction on CIP, phenol, BHA, and coumarin reach 54.96%/39.47%, 33.43%/24.79%, 35.29%/20.14%, and 40.13%/22.97%, respectively. The polarization charge of Ag is used to modulate Fermi level of BiVO+4 and g-C3N4 semiconductors to form crystalline S-type heterojunctions on the BiVO4 (010) crystalline surface to enhance the redox capability and broad-spectrum degradation of photocatalysts in the full spectral range. [ABSTRACT FROM AUTHOR]