<p>This study explores the dual functionality of α-MnO₂ and Cr/Ni-doped α-MnO₂ as photocatalysts for dye degradation and as electrode materials for supercapacitors. α-MnO₂ was synthesized using a green approach involving <i>Aloe vera</i> extract, and Cr/Ni doping was achieved via the addition of chromium and nickel precursors. Structural, morphological, and surface analyses confirmed successful doping, lattice expansion, and the introduction of oxygen vacancies, leading to enhanced performance. Photocatalytic tests showed a 47% increase in dye degradation rate for Cr/Ni-doped α-MnO₂ compared to pristine α-MnO₂ under visible light. Electrochemical evaluation revealed a significant improvement in specific capacitance, from 150 F/g for α-MnO₂ to 230 F/g for Cr/Ni-doped α-MnO₂, attributed to enhanced conductivity and active sites introduced by doping. The findings demonstrate the versatility of these materials in environmental remediation and energy storage applications, offering a promising pathway for multifunctional material design.</p>