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Urine source separation, as an innovative concept for the reuse of microlevel nutrients in human urine, has drawn increasing attention recently. Consequently, removing coexisting pharmaceuticals in urine is necessary for further reuse. This study is the first to apply the solar-driven persulfate process (Solar/PS) to the investigation of cephradine (CFD) and caffeine (CAF) degradation in synthetic human urine. The results showed that significantly more degradation of CFD and CAF occurs with the Solar/PS process than with persulfate oxidation and direct sunlight photolysis, respectively. The generated reactive species ·OH, SO 4 ·–, O 2 ·– and 1O 2 were identified in the Solar/PS process. While SO 4 ·– played a dominant role at pH 6, it played a minor role at pH 9 due to the lower amount generated under alkaline conditions. The presence of chloride and ammonia negatively impacted the photodegradation of both compounds. In contrast, bicarbonate exhibited no effect on CAF but enhanced CFD degradation owing to its amino-acid-like structure, which has a higher reactivity toward CO 3 ·–. Although total organic carbon (TOC) was partially mineralized after 6 h of operation, no Microtox® toxicity was observed. [Display omitted] • CAF and CFD were effectively removed in synthetic urine via the Solar/PS process. • SO 4 ·– contributed dominantly at pH 6, while·OH played a major role at pH 9. • Cl- and NH 3 in synthetic urine had a negative impact on CAF and CFD degradation. • HCO 3 - in synthetic urine exhibited no effect on CAF but enhanced CFD degradation. • No Microtox® toxicity was observed in synthetic urine after the operation. [ABSTRACT FROM AUTHOR]