We report on two pairs of platinum acetylide based polymers and model oligomers utilizing a 2,1,3-benzothiadiazole (BTD) acceptor moiety flanked on either side by either 2,5-thienyl donor units (Pt 2 BTD-Th and p-PtBTD-Th) or (3,4-ethylenedioxy)-2,5-thienyl donors (Pt 2 BTD-EDOT and p-PtBTD-EDOT). Both oligomer/polymer pairs absorb strongly throughout the visible region; however, because the (ethylenedioxy)thiophene moiety is a stronger donor than thiophene, the latter oligomer/polymer pair has a correspondingly lower band gap and, therefore, harvests light more efficiently at longer wavelengths. p-PtBTD-Th exhibits a relatively narrow molecular weight distribution with a number-average molecular weight (M n) of 22 kDa, while p-PtBTD-EDOT exhibits a comparable M n of 33 kDa but has a high polydispersity index likely due to aggregation. We provide a complete report of the photophysical and electrochemical characterization of the two oligomer/polymer pairs. The photophysical studies reveal that the materials undergo relatively efficient intersystem crossing. In a discussion of the energetics of photoinduced electron transfer from the platinum polymers to [6,6]-phenyl C 61 butyric acid methyl ester (PCBM), it is noted that while the singlet state is quenched efficiently, the triplet state is not quenched, indicating that charge generation in the photovoltaic materials must ensue from the singlet manifold. Finally, organic photovoltaic devices based on blends of p-PtBDT-Th or p-PtBDT-EDOT with PCBM were characterized under monochromatic and simulated solar (AM1.5) illumination. Optimized devices exhibit an open-circuit voltage (V oc) of ∼0.5 V, a short-circuit current density (I sc) of ∼7.2 mA cm -2 , and a fill factor of ∼35%, which yields overall power conversion efficiencies of 1.1-1.4%.