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One two‐dimensional (2D) GdIII coordination polymer based on isonicotinic acid N‐oxide (HINNO), {[Gd(INNO)2(HCOO)] ⋅ 2H2O}n (1), was successfully synthesized and characterized. Magnetic studies reveal the presence of weak antiferromagnetic couplings between adjacent GdIII ions in the 1D chain units of 1 and large cryogenic magnetocaloric effect with maximum −ΔSm of 31.84 J kg−1 K−1 at T=2 K and ΔH=7...