In this work, the author developed Ca4Fe9O17/biochar (CFB) via a green method through a facile co-precipitation procedure involving egg shells as calcium precursor and investigating its performance in single as well as binary solution of methylene blue (MB) and rhodamine B (RhB). The CFB nanocomposite was characterized by XRD, SEM, TEM, XPS, Raman, FTIR, BET, and VSM. ESR studies show the presence of hydroxyl (·OH) and superoxide (O2·¯) radicals, which are primary radical species for pollutant degradation. The average crystalline size of CFB nanocomposites was found to be 32.992 nm using XRD, whereas TEM analysis indicates a particle diameter of 35–36 nm. The degradation efficacy of MB and RhB dyes was achieved at 99.2% and 98.6%, respectively, in a single solution, whereas 99.4% and 99.2%, respectively, in a binary solution within 36 min. Additionally, an iron cluster was formed during the degradation process of MB dye. The degradation of organic contaminants and generation of iron clusters from the degraded dye products were both expedited by the remarkable extension effect of the Ca4Fe9O17 in the CFB nanocomposites. The three processes were achieved using CFB nanocomposite: (1) the advanced oxidation process; (2) degradation of MB and RhB dye in single as well as binary solution with enhanced efficiency, (3) the production of the iron cluster from degraded products. Thus, these three steps constitute a smart and sustainable way that leads to an effective effluent water treatment system and the generation of iron clusters preventing secondary pollution.