A series of solid solutions of indium and iron oxides with different In/Fe ratios (InxFeyO3, with x + y = 2) were synthesized in the form of nanoparticles with the purpose of generating semiconductors with an intermediate band gap width compared to those of In2O3 and Fe2O3. XRD analysis proved the formation of the desired InxFeyO3 solid solutions for Fe content in the range 5-25% mol. UV-Vis absorption analysis showed that the substitution of In with Fe in the crystalline structure led to the anticipated gradual decrease of the band gaps energy values compared to In2O3. The obtained materials were tested as photocatalysts for the degradation of model organic pollutants (phenol and methylene blue) in water. Among the InxFeyO3 solid solutions, In1.7Fe0.3O3 displayed the highest photocatalytic activity in the degradation of the selected probe molecules under UV and visible radiation. Remarkably, In1.7Fe0.3O3 showed a significantly enhanced activity under visible light compared to monometallic indium oxide and iron oxide. This demonstrates that our strategy consisting in engineering the band gap by tuning the composition of InxFeyO3 solid solutions was successful in improving the photocatalytic performance under visible light. Additionally, In1.7Fe0.3O3 fully retained its photocatalytic activity upon reuse in four consecutive cycles.