The mass production and widespread use of pharmaceuticals and personal care products (PPCPs) posed a great threat to the water environment and human health. In this paper, a green plant-based Bi-Zr bimetallic MOF SU-101.2 was prepared, and the adsorption characteristics were studied with typical PPCPs-Diclofenac sodium (DCF). Compared to SU-101 and SU-102, SU-101.2 showed a significant increase in the adsorption rate of DCF. The adsorption mechanisms between SU-101.2 and DCF were mainly electrostatic interactions, hydrogen bonding and π-π interactions. Moreover, SU-101.2 also had considerable photocatalytic properties, which was applied to the subsequent treatment of adsorbent desorption, effectively solving the problem of secondary pollution and achieving a green sustainable adsorption and degradation cycle. In all, this work presented an effective adsorbent and a sustainable approach for DCF elimination, which could replace traditional chemical desorption and regenerate the adsorbent via a photocatalytic process.