In this paper, two compounds [Zn₂²⁺(2,6-bis(4΄-pyridyl)-TTF)(TPA)₂^2-] (1) and [Cd²⁺(2,6(7)-bis(4΄-pyridyl)-TTF)(TPA)^2-(H₂O)₂] (TTF = tetrathiafulvalene, TPA = terephthalic acid) (2) were synthesized by using solvothermal method and characterized by single-crystal X-ray. The purity of the two compounds was confirmed by their PXRD data. We also tested the photocurrent responses of these two compounds, and found they could generate photocurrent signal when exposed to light, but the photocurrent intensity of compound 2 is significantly greater than that of 1. From the crystal structure analysis, the possible reason for this phenomenon is that 2 has a more compact ligand arrangement than 1, leading to a higher carrier density and easier excitation.