A solvent free synthetic method using rice husk ash (RHA) as solid support has been designed for selective functionalization and preparation of novel 1,1′- unsymmetrically bi-functionalized ferrocenyl compounds. The selectively functionalized intermediate compound, Ferrocenyl-1-acetyl-1′-thiosemicarbazone, has been structurally characterized using single crystal X-ray diffraction technique which revealed distinct inter-molecular hydrogen bonding interactions across the thiosemicarbazone chains. Cytotoxic evaluation of five different unsymmetrically bi-functionalized thiosemicarbazone - hydrazone compounds showed potent activity against human leukemia (THP-1) cell line. The unsymmetrical ferrocenyl compounds also showed strong BSA and DNA binding interactions and reversible redox properties.