Thiosemicarbazones are known for their versatile coordination behavior and wide-ranging applications in the fields of materials science, catalysis, and medicinal chemistry. Metal complexes of thiosemicarbazones are extensively studied because of their remarkable properties and diverse applications in various scientific disciplines. Several investigations have reported on the biological potential of transition metal complexes of TSCs, including antifungal, antiviral, antibacterial, and anticancer activities. Studies on heterocyclic TSC complexes have become more prevalent. In addition, the structural, electronic, and reactive properties of these complexes are explored through computational studies using molecular docking and density functional theory (DFT). Such investigations not only support the interpretation of experimental results but also influence synthetic design by predicting the structural behavior of the complexes. Moreover, these computational techniques enable researchers to examine electronic structures and spectroscopic characteristics, which are crucial for establishing Structure–Activity Relationships (SARs) and understanding reactivity patterns. The gap between experimental research and theoretical understanding is bridged by computational studies, enabling the behavior of metal complexes in various biological and chemical systems to be predicted and optimized. The design and development of more effective compounds for various applications is made easier by this approach. In this study, we explore computational studies of thiosemicarbazone metal complexes along with their biological activities.