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Four new Schiff-base type conjugative polymers (CPs), that is, Py 1-4 carrying a strong electron-withdrawing cyanopyridine scaffold coupled with different electrondonating aromatic/heteroaromatic moieties were synthesized from their respective co-monomers by simple poly-condensation route. They were subjected to structural, thermal, photophysical, and electrochemical characterizations and theoretical investigations in order to identify their suitability in polymer light-emitting diode (PLED) application. All these polymers showed good film-forming ability and exhibited favorable photophysical behaviors with an optical bandgap in the order of 2.54-2.68 eV. Further, their electrochemical data were used to evaluate highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels. Finally, Py 1-4 were successfully employed as blue-light emitter in the construction of new ITO/PEDOT:PSS/ Py 1-4 /Al configured light-emitting diodes (LED), and the fabricated devices demonstrated stable blue electroluminescence behavior endorsing an effective electrons injection in the PLEDs.