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The construction of multifunctional metal-organic frameworks (MOFs) has attracted considerable attention. Two novel Dy-MOFs namely [Dy2(TPTC-2OMe)1.5(H2O)4·H2O]n (1) and {[Dy2(TPTC-2OMe)(H2TPTC-2OMe) (H2O)2]·2H2O}n (2) were obtained by a solvothermal method using 2′,5′-dimethoxy-[1,1′:4′,1″-terphenyl]- 4,4″-dicarboxylic acid (H4TPTC-2OMe) as the ligand. Structure analysis demonstrates that both MOFs 1 and 2 displayed three-dimensional framework structures, in which MOF 1 was with Dy(III) metal chains as nodes, while MOF 2 was with Dy2 binuclear metal clusters as nodes. Interestingly, MOFs 1 and 2 exhibited high thermal and chemistry stabilities and presented relatively high proton conductivity (σ) values of 1.69 × 10-4 S cm-1 and 3.52 × 10-6 S cm-1 at 50 °C and 98% RH. Although there exist a large number of coordinated or free H2O molecules in both structures, it is easier to form an ordered hydrogen-bonding network between the coordinated H2O molecules in the structure of MOFs, resulting in a more excellent proton conductivity of MOF 1. Moreover, MOF 1 exhibited field-induced single-molecule magnet (SMM) behavior with energy barriers (Ueff) of 37.22 K (τ0 = 9.27 × 10-8 s). Furthermore, MOF 1 exhibits obvious second-order nonlinear optical properties. This research provides guidance for the design of novelty multifunctional MOF materials. [ABSTRACT FROM AUTHOR]