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In an attempt to develop new coloured inorganic oxides, we have investigated the substitution of 3d transition‐metal ions in LiMgBO3 host [where MgII has a trigonal bipyramidal (TBP) oxygen coordination]. We find that single‐phase materials are formed for LiMg1–xCoIIxBO3 (0 < x ≤ 1.0), LiMg1–xNiIIxBO3 (0 < x ≤ 0.1), LiMg1–xCuIIxBO3 (0 < x ≤ 0.1) and also Li1–xMg1–xFeIIIxBO3 (0 < x ≤ 0...