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We report the effect of substitution of Ru by Ta in Sr2YbRuO6 on its magnetic and photoelectrocatalytic properties. The powder X-ray diffraction data, was satisfactorily refined in the monoclinic space group, P21/n. The DC magnetization studies indicated that Sr2YbRuO6 shows antiferromagnetic interaction through Yb–O–Ru orbital ordering, with the highest Weiss temperature, among Sr2YbRu1–x Ta x O6 (x = 0, 0.25, 0.5, and 0.75) which have values of −148, −125, −118, and −102 K, respectively. The difference in observed and theoretical magnetic moments was found to increase as x increases. It was also observed that with the increase of Ta concentration in Sr2YbRu1–x Ta x O6, the band gap increased almost linearly, from 1.78(1) eV (x = 0) to 2.08(1) (x = 0.75), and thereafter a sharp increase 2.65(1) eV (x = 1) was observed, with the lowering of energy level of valence band, along with disruption in orbital ordering as x increases. The photoelectrocatalytic oxygen evolution reaction (OER) studies carried out on the series yield a maximum photocurrent density of 17 μA/cm2 and photoresponse current of 5.5 μA/cm2 at 0.8 V at an onset potential at 0.29 V vs Ag/AgCl for Sr2YbRuO6. The XPS analysis showed Ta and Ru to be in +5/+4 oxidation states, with the highest concentration of Ru4+ ion observed for Sr2YbRuO6. The presence of oxygen vacancies was confirmed by XPS as well as EPR studies.