A one-dimensional (1D) chain compound (en = ethylenediamine), featuring tetrahedral FeSe2 chains separated by [Fe(en)(3)] cations and Cl anions, has been synthesized by a low temperature solvothermal method using simple starting materials. The degree of distortion in the FeSe backbone is similar to previously reported compounds with isolated 1D FeSe chains. Fe Mossbauer spectroscopy reveals the mixed-valent nature of [Fe(en)](3)(FeSe2)(4)Cl-2 with Fe3+ centers in the [FeSe]- chains and Fe2+ centers in the [Fe(en)] complexes. SQUID magnetometry indicates that is paramagnetic with a reduced average effective magnetic moment, mu eff = 9.51 mu B per formula unit, and a negative Weiss constant, ? = -10.9(4) K, indicating antiferromagnetic (AFM) nearest neighbor interactions within the [FeSe2]- chains. Weak antiferromagnetic coupling between chains, combined with rather strong intrachain AFM coupling, leads to spin-glass behavior at low temperatures, as indicated by a frequency shift of the peak observed at 3 K in AC magnetic measurements. A combination of [Fe(en)] and Cl ions is also capable of stabilizing mixed-valent 2D FeSe puckered layers in the crystal structure of [Fe(en)(3)]4(Fe14Se21)Cl-2, where Fe14Se21 layers have a unique topology with large open pores. Property measurements of [Fe(en)3]4(Fe14Se21)Cl-2 could not be performed due to the inability to either grow large crystals or synthesize this material in single-phase form.