In our previous research, varying Ni concentration in a Mg-doped CuCrO \(_2\) matrix enhanced the Seebeck coefficient via carrier–magnon drag, but the overall power factor remained low. In this work, a modified synthesis strategy and precise dopant control enabled the decoupling of thermoelectric parameters, enhancing carrier mobility through Mg \(^{2+}\) -induced potential barriers in Ni \(^{2+}\) -doped CuCrO \(_2\) . X-ray diffraction (XRD) confirms the incorporation of Mg \(^{2+}\) and structural modifications, while vibrating sample magnetometry (VSM) reveals Ni \(^{2+}\) -driven collinear spin ordering in the frustrated CuCrO \(_2\) lattice. Magnetoresistance studies further elucidate the interaction between non-magnetic Mg \(^{2+}\) and magnetic ordering, shedding light on its impact on transport behavior. This structural and magnetic reconfiguration enhances spin entropy, contributing to an increased Seebeck coefficient (317 \(\mu\) V/K) and electrical conductivity (6779 S/m) at 700 \(^\circ\) C. The interplay of these effects results in a record-high power factor (0.722 mW/mK \(^2\) ) among Cu-based delafossites. In addition, thermal conductivity measurements confirm a reduced \(\kappa\) of 2.84 W/mK, attributed to increased phonon scattering at Mg-induced interfaces. This study provides direct experimental evidence of interlamellar porosity and spin-driven transport mechanisms, offering new insights into structural tuning for high-performance thermoelectrics.
