The use of chemical materials to tackle environmental concerns has undergone significant evolution, particularly in the pursuit of strategies for removing pollutants from wastewater as part of environmental remediation an increasingly crucial research topic. Employing green photocatalysts stands out as an efficient and cost-effective approach, playing a key role in promoting sustainable environmental remediation. This study introduces the modification of zinc oxide with cobalt chromite (CoCr2O4/ZnO) through a green synthesis method employing Basella alba L. leaves extract (BALE). Utilizing various characterization techniques, including FT–IR, UV–Vis DRS, XRD, SEM-EDS, and TEM, key features of ZnO, CoCr2O4, and CoCr2O4/ZnO nanocomposites were identified. The optical band gaps for ZnO, CoCr2O4, and CoCr2O4/ZnO nanocomposites were determined as 3.16, 1.71, and 2.80 eV, respectively, where it was shown that the band gap of the ZnO was reduced significantly. CoCr2O4/ZnO nanocomposites displayed a cubic shape of CoCr2O4 on the surface of ZnO, with a particle size of 23.84 ± 8.08 nm. The photocatalytic activity was assessed through the degradation of malachite green under visible light irradiation, where the CoCr2O4/ZnO nanocomposites exhibited superior photodegradation efficiency at 90.91%, surpassing ZnO alone (57.09%). This improvement in photocatalytic activity is attributed to a reduced band gap energy and a high rate constant value of 9.57 × 10−3 min−1, demonstrating pseudo-first-order reaction kinetics. In summary, this research presents the development of a ZnO-based photocatalyst with exceptional performance, especially in the visible light spectrum, making it a promising candidate for applications in wastewater removal.