One novel metal organic framework {[Ni-6(OH)(4)(BTB)(8/3)(H2O)(6)]center dot 4H(2)O center dot 9DMF}(n) (DMF = dimethylformamide) based on 1,3,5-benzenetribenzoic acid (H3BTB) was successfully synthesized under basic condition at room temperature, featuring a unique twofold interpenetrated pcu-type net with [Ni-6(OH)(4)(COO)(8-)(H2O)(6)] cluster as building block. Its gas-adsorption behaviors were investigated and modified by utilizing metal(II)-doped procedure, which was certified to be a highly effective pathway in enhancing CO2 uptake capacity.