This study investigates the role of metals in the adsorption and photodegradation of glyphosate (GP) using four metal-organic frameworks (MOFs): Sc-TBAPy, Al-TBAPy, Y-TBAPy, and Fe-TBAPy. Sc-TBAPy demonstrated superior performance in both GP adsorption and degradation. Under light irradiation for 5 minutes, Sc-TBAPy completely degraded 100% of GP in a 1.5 mM aqueous solution. Femtosecond transient absorption spectroscopy revealed that Sc-TBAPy has enhanced charge transfer properties and suppressed formation of emissive excimers, which could hinder photocatalysis. Hydrogen evolution half-reaction experiments confirmed Sc-TBAPy's superior catalytic activity for water splitting. Sc-TBAPy also exhibited a selective pathway for GP oxidation, avoiding the formation of toxic aminomethylphosphonic acid (AMPA), unlike other MOFs. Electron spin resonance, depleted oxygen conditions, and solvent exchange with D₂O were used to study the role of reactive oxygen species (ROS) in GP photodegradation. Singlet oxygen (¹O₂) was identified as a key factor in the selective photodegradation pathway of Sc-TBAPy. GP is a widely used herbicide with potential health risks, including increased cancer risk and developmental defects. Its persistence in soil and water sources poses environmental concerns. Bacterial degradation pathways include GP oxidoreductase and C–P lyase, with the latter being more desirable. However, microbial degradation is limited by environmental factors. Adsorbents like activated carbon and graphene oxide can remove GP but have limitations in recovery and efficiency. Oxidative processes such as photo-Fenton and electro-Fenton can degrade GP but often produce toxic byproducts like AMPA. Photocatalysis is promising due to its mild conditions and selectivity. Sc-TBAPy, a pyrene-based MOF, showed high efficiency in GP degradation, with Sc-TBAPy outperforming other MOFs in adsorption and degradation. The study highlights the importance of metal-ligand synergy in MOF design for efficient GP removal. Sc-TBAPy's superior performance is attributed to its enhanced charge transfer, efficient ROS generation, and selectivity in GP degradation. The findings suggest that MOFs can be tailored for selective and efficient removal of organic pollutants from water.This study investigates the role of metals in the adsorption and photodegradation of glyphosate (GP) using four metal-organic frameworks (MOFs): Sc-TBAPy, Al-TBAPy, Y-TBAPy, and Fe-TBAPy. Sc-TBAPy demonstrated superior performance in both GP adsorption and degradation. Under light irradiation for 5 minutes, Sc-TBAPy completely degraded 100% of GP in a 1.5 mM aqueous solution. Femtosecond transient absorption spectroscopy revealed that Sc-TBAPy has enhanced charge transfer properties and suppressed formation of emissive excimers, which could hinder photocatalysis. Hydrogen evolution half-reaction experiments confirmed Sc-TBAPy's superior catalytic activity for water splitting. Sc-TBAPy also exhibited a selective pathway for GP oxidation, avoiding the formation of toxic aminomethylphosphonic acid (AMPA), unlike other MOFs. Electron spin resonance, depleted oxygen conditions, and solvent exchange with D₂O were used to study the role of reactive oxygen species (ROS) in GP photodegradation. Singlet oxygen (¹O₂) was identified as a key factor in the selective photodegradation pathway of Sc-TBAPy. GP is a widely used herbicide with potential health risks, including increased cancer risk and developmental defects. Its persistence in soil and water sources poses environmental concerns. Bacterial degradation pathways include GP oxidoreductase and C–P lyase, with the latter being more desirable. However, microbial degradation is limited by environmental factors. Adsorbents like activated carbon and graphene oxide can remove GP but have limitations in recovery and efficiency. Oxidative processes such as photo-Fenton and electro-Fenton can degrade GP but often produce toxic byproducts like AMPA. Photocatalysis is promising due to its mild conditions and selectivity. Sc-TBAPy, a pyrene-based MOF, showed high efficiency in GP degradation, with Sc-TBAPy outperforming other MOFs in adsorption and degradation. The study highlights the importance of metal-ligand synergy in MOF design for efficient GP removal. Sc-TBAPy's superior performance is attributed to its enhanced charge transfer, efficient ROS generation, and selectivity in GP degradation. The findings suggest that MOFs can be tailored for selective and efficient removal of organic pollutants from water.