Recent studies on next-generation permanent magnets have focused on filling in the gap between rare-earth magnets and rare-earth-free magnets, taking into account both the cost-effectiveness and magnetic performance of the magnetic materials. As an improved rare-earth-free magnet candidate, here, Ca-substituted M-type Sr-lean hexaferrite particles within a nano- to micro-scale regime, produced using an ultrasonic spray pyrolysis method, are investigated. Theoretically, the maximum coercivity (Hc) can be achieved in submicron Sr-ferrite crystals (i.e., 0.89 μm). The plate-like resultants showed a significant enhancement in Hc, up to a record high of 7880.4 Oe, with no deterioration in magnetization (M: 71-72 emu/g). This resulted in more favorable magnetic properties than those of the traditional Sr-La-Co ferrites. On the basis of microstructural analysis and fitting results based on the law of approach to saturation method, the Ca-substitution effects on the change in size and anisotropic characteristics of the ferrite particles, including pronounced lateral crystal growth and a strong increase in magnetocrystalline anisotropy, are clearly demonstrated. The cost-effective, submicron, and Ca-substituted Sr-ferrite is an excellent potential magnet and moreover may overcome the limitations of traditional hard magnetic materials.