The quest to enhance solar cell performance has long been driven by increasing energy demands and environmental concerns, and much progress has been achieved by way of interface modifications. As the demand for sustainable energy increases and environmental awareness pushes us toward cleaner solutions, the spotlight turns on stable and eco-friendly metal oxide semiconductors for photovoltaic applications. This research highlights the exceptional electronic and optical characteristics of ZrO2@GO nanoparticles, focusing on molecular electrostatic potential (MEP), nonlinear optical properties (NLO), and electron localization function (ELF). Our findings highlight that ZrO2@GO exhibits superior electronic characteristics compared to bare graphene oxide. This superiority motivates us for the co-sensitization of ZrO2@GO with Squaraine dyes, which are well known for their strong light harvesting in dye-sensitized solar cells (DSSC). Using density functional theory (DFT) with Gaussian 09, we examine critical parameters that include the highest occupied molecular orbital (HOMO), lowest unoccupied molecular orbital (LUMO), energy gap, maximum wavelength (λmax), electron injection efficiency (ΔGinject), open-circuit voltage (Voc), reorganization energy (λreorg), among others. Our research highlights the high optical transmittance of ZrO2@GO, positioning it as a promising material for advanced optical, electrical, and light-harvesting devices with improved performance and efficiency.