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Attempts to crystallize Cu(2,6-dmpz)(NO3)2 (2,6-dmpz = 2,6-dimethylpyrazine) by reaction of 2,6-dmpz with Cu(NO3)2· 3H2O in THF resulted in the synthesis of Cu(2,6-dmpz)2(NO3)2· THF. The compound crystallized in the monoclinic space group C2/c and exists as isolated molecules with distorted square pyramidal geometry: a = 11.609(4) Å, b = 10.415(3) Å, c = 18.256(6) Å, β = 108.332(4)°. The 2,6-dmpz molecules coordinate to the Cu ions through the distal (remote from the methyl) nitrogens. The molecules are arrayed in stacks parallel to the b-axis.