The synthesis and characterization of five novel organonickel-organosilicon alternating copolymers having the repeating unit - C6F4 - Ni(PBu(3))(2) - C6F4 - SiR(2) - [where SiR(2) = SiMe(2) -, - SiMe (Hex) -, - SiPh(2) -, -- SiMe(2) - O - SiMe(2) -, and - SiMe(2) - (CH2) (6) - SiMe(2)-] are reported. The model compounds Ni(PR(3))(2)(1,4C(6)F(4)SiMe(3))(2) (PR(3) = PMePh(2) or PBu(3)) were prepared via reactions of Ni(PR(3))(2)( 1,4-C6F4Li)(2) with 2 equiv of SiMe(3)Cl, and were characterized by conventional analytical and spectroscopic measurements. The polymers were prepared from the reactions of Ni(PBu(3))(2)(1,4-C6F4Li)(2) with 1 equivalent of SiMe(2)Cl(2) (polymer 1, M ($) over bar omega = 15,800), SiMe(Hex) Cl-2 (polymer 2, M ($) over bar omega = 7300), SiPh(2)Cl(2) (polymer 3, M ($) over bar omega = 8600), O(SiMe(2)Cl)(2) (polymer 4, M ($) over bar omega = 13,900) and (CH2)(6)(SiMe(2)Cl)(2) (polymer 5, M ($) over bar omega = 19,700). The molecular weights for each polymer were fully determined by both GPC and VPO. The multinuclear (H-1-, F-19-, and P-31 {H-1})- NMR, FTIR, and UV-Visible spectroscopic data for each polymer unambiguously establishes its repeating unit structure. The observations indicate that introduction of the silyl or siloxane units into the organonickel backbones has remarkably decreased the chain rigidity of the organonickel-organosilicon polymers compared to their rigid rod organonickel analogues(i.e., - [ - C6F4 - Ni(PR(3))(2) -](n) -).