For the last four decades, researchers’ intense attentions have been received on transition-metal oxide-doped semiconductors. The substitution of transition metals on a host element adds the local magnetic moment to the system’s low-energy degree of freedom pave way for spintronics, i.e., spin electronics. So the existing semiconductors with magnetic impurities are known to be dilute magnetic semiconductors (DMSs). DMS mainly focuses on II–VI (ZnO, TiO2), IV–VI (PbTe, SnTe), and recently III–V (GaAs, InSb) semiconductors doped with transition-metal (TM) ions (Mn, Fe, Co, Ni, Cu, etc.). The realistic concerns on spintronic materials are (i) materials should retain the ferromagnetic property above room temperature and (ii) should have promising advantages over the existing technologies. It is the discovery of giant magnetoresistance (GMR) that triggered the investigations on spintronic devices. Considering the tremendous optical and magnetic properties of transition-metal oxides (TMOs), design and development of TMO-based spintronic devices are increasing day by day in comparison with non-oxide semiconductors. More importantly, ZnO claims room temperature ferromagnetism and much isolated transport properties. ZnO-based DMS materials have recently attracted much interest for its ease in band gap tuning with the addition of suitable dopants. In addition to magnetic ion doping and additional charge carriers, the ferromagnetic ordering occurs through indirect exchange interaction, RKKY interaction mediated through electrons (n-type) or holes (p-type) through the valence band of ZnO. Longer-range ferromagnetic exchange can be mediated by carriers in a spin-polarized band. ZnO-based spintronic devices can be successfully brought into fruition with the ability to create and control spin-polarized charge carrier transport. Even though a large number of researches are going on globally, achieving a higher transition temperature is still a challenging problem. Theoretical works like first principle studies give an insight to the underlying physics of these phenomena to some extent. There also lie some mismatches in predicting the oxidation states and electronic structure which could adversely affect the predicted magnetic properties when made it practical. Researchers used a self-interaction-corrected local density approximation (LDA) approach to carry out the calculations on ZnO-based DMS and presented a systematic comparison between the studies carried out within self-interaction-corrected LDA and standard LDA. The most commonly occurring experimental limitations in SQUID measurements are artifices arising from improper sample handling. The major factors to be analyzed during growth parameters include substrate effects, influence of post annealing and formation of secondary phases and effect of dopants are to be dealt with. So this chapter will give an insight of the correlation of various experimental results on ZnO-based DMS and with supporting theories and ab initio calculations.