A new n = 2 Ruddlesden-Popper (RP) series La2SrFe2-xCrxO7 (x = 0.0, 0.2, 0.4, 0.6 and 0.8) has been prepared via Sol-gel Pechini method, and their structural, optical, and the magnetic characterization was done. Furthermore, we are for the first-time reporting on the photo-catalytic degradation of a dye by a complete n = 2, La2SrFe2-xCrxO7 RP series. Rietveld refinement analysis confirms the formation of single-phase compounds with tetragonal crystal symmetry and I4/mmm space group. The results indicate a steady decrease in unit cell parameters and cell volume with Cr3+ doping. Dominant anti-ferromagnetic (AFM) interactions were observed in all the phases and the appearance of weak ferromagnetic (FM) interactions takes place owing to the Fe3+―O―Cr3+ FM interaction with Cr3+ doping. The χM−FC curve for x = 0.8 phase shows the magnetization reversal (MR) phenomenon and becomes zero at Tcomp ∼127 K and the value becomes negative on further decreasing the temperature. The MR phenomenon is discussed in terms of the competing Fe3+―O―Fe3+, Fe3+―O―Cr3+, and Cr3+―O―Cr3+ super-exchange interactions. Enhanced photocatalytic activity for the degradation of Rhodamine B (RhB) dye was obtained for x = 0.2 substituted phase, displaying a ∼99% degradation of dye in 30 min followed by ∼83%, ∼75%, ∼64% and ∼61% by x = 0.4, 0.0, 0.8 and 0.6 phases respectively in the same time interval. The results are explained in terms of crystallite size, the narrowing of band gap with Cr3+ substitution, and based on of recombination of charge carriers which, are in good agreement with the results of Photoluminescence (PL) emission intensity spectra.