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In the quest to combat global warming, traditional thermal chemistry processes are giving way to selective photocatalysis, an eco-friendly approach that operates under milder conditions, using benign solvents like water. Benzaldehyde, a versatile compound with applications spanning agroindustry, pharmaceuticals, and cosmetics, serves as a fundamental building block for various fine chemicals. This study aims at enhancing benzaldehyde production sustainability by utilizing photooxidation of benzyl alcohol. Gold nanoparticle-based catalysts are renowned for their exceptional efficiency in oxidizing bio-based molecules. In this research, Au nanoparticles were anchored onto three distinct supports: <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi mathvariant="normal">T</mi><mi mathvariant="normal">i</mi><msub><mi mathvariant="normal">O</mi><mn>2</mn></msub></mrow></semantics></math></inline-formula>, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi mathvariant="normal">Z</mi><mi mathvariant="normal">r</mi><msub><mi mathvariant="normal">O</mi><mn>2</mn></msub></mrow></semantics></math></inline-formula>, and graphitic carbon nitride (g-<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi mathvariant="normal">C</mi><mn>3</mn></msub><msub><mi mathvariant="normal">N</mi><mn>4</mn></msub></mrow></semantics></math></inline-formula>). The objective was to investigate the influence of the support material on the selective photocatalysis of benzyl alcohol. In the preparation of g-<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi mathvariant="normal">C</mi><mn>3</mn></msub><msub><mi mathvariant="normal">N</mi><mn>4</mn></msub></mrow></semantics></math></inline-formula>, three different precursors—melamine, urea, and a 50:50 mixture of both—were chosen to analyze their impact on catalyst performance. After 4 h of irradiation at 365 nm, operating under acidic conditions (pH = 2), the Au photocatalyst on graphitic carbon nitride support synthesized using urea precursor (Au@g-<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi mathvariant="normal">C</mi><mn>3</mn></msub><msub><mi mathvariant="normal">N</mi><mrow><mn>4</mn><mo>(</mo><mi>u</mi><mi>r</mi><mi>e</mi><mi>a</mi><mo>)</mo></mrow></msub></mrow></semantics></math></inline-formula>) displayed the optimal balance between conversion (75%) and selectivity (85%). This formulation outperformed the benchmark Au@TiO₂, which achieved a similar conversion rate (80%) but exhibited lower selectivity (55%).