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A new dinuclear europium cluster (Eu-cluster) is synthesized and the exact structure is determined by single-crystal X-ray diffraction. The formula of the Eu-cluster is determined to be [Eu 2 (4-Msal) 6 (phen) 2 (H 2 O) 2 ] (4-Msal = 4-methylsalicylic acid, phen = phenanthroline), it crystallizes in the triclinic space group P -1, with a = 9.1193(8) Å, b = 13.0855(10) Å, c = 14.0981(9) Å, α = 103.159(6)°, β = 94.192(6)°, γ = 100.632(7)°, V = 1598.3(2) Å 3 and Z = 1. Further investigation reveals that the Eu-cluster is a highly sensitive and selective methylmercury (CH 3 Hg + ) sensor. To the best of our knowledge, this is the first CH 3 Hg + sensor based on lanthanide clusters/complexes. The responsive behavior shows the sensing has excellent linearity in 1.4–3.8 μg L −1 μM. The LOD for sensing CH 3 Hg + is 0.8 μg L −1 , which meets the standard of Chinese environmental quality standard for agricultural and industrial water. Interestingly, study also reveals the sensor is applicable in real water sensing. [ABSTRACT FROM AUTHOR]