Perovskite solar cells (PSCs) have emerged as promising photovoltaic technologies owing to their high power conversion efficiency (PCE) and material versatility. Conventional optimization of PSC architectures largely depends on iterative experimental approaches, which are often labor-intensive and time-consuming. In this study, a data-driven modeling strategy is introduced to accelerate the design of efficient and mechanically robust PSCs. Seven supervised regression models were evaluated for predicting key photovoltaic parameters, including PCE, short-circuit current density (Jsc), open-circuit voltage (Voc), and fill factor (FF). Among these, a stacking ensemble framework exhibited superior predictive accuracy, achieving an R² of 0.8577 and a root mean square error of 2.084 for PCE prediction. Model interpretability was ensured through Shapley Additive exPlanations(SHAP) analysis, which identified precursor solvent composition, A-site cation ratio, and hole-transport-layer additives as the most influential parameters. Guided by these insights, ten device configurations were fabricated, achieving a maximum PCE of 24.9%, in close agreement with model forecasts. Furthermore, multiscale mechanical assessments, including bending, compression, impact resistance, peeling adhesion, and nanoindentation tests, were conducted to evaluate structural reliability. The optimized device demonstrated enhanced interfacial stability and fracture resistance, validating the proposed predictive–experimental framework. This work establishes a comprehensive approach for performance-oriented and reliability-driven PSC design, providing a foundation for scalable and durable photovoltaic technologies.

Perovskite solar cells (PSCs) rarely report, on a single-device platform, concurrent gains in optoelectronic efficiency and buried-interface mechanical robustness—two prerequisites for flexible and roll-to-roll (R2R) integration. We engineered a nanoplate-structured fluorine-doped tin oxide (NP-FTO) front electrode that couples light management with three-dimensional interfacial anchoring, and we quantified both photovoltaic (PV) and nanomechanical metrics on the same device stack. Relative to planar FTO, the NP-FTO PSCs achieved PCE of up to 25.65%, with simultaneous improvements in Voc (to 1.196 V), Jsc (up to 26.35 mA cm⁻²), and FF (to 82.65%). Nanoindentation revealed a ~28% increase in reduced modulus and >70% higher hardness, accompanied by a ~32% reduction in maximum indentation depth, indicating enhanced load-bearing capacity consistent with the observed FF gains. The low-temperature, solution-compatible NP-FTO interface is amenable to R2R manufacturing and flexible substrates, offering a unified route to bridge high PCE with reinforced interfacial mechanics toward integration-ready perovskite modules.