The rapid evolution of materials informatics provides scalable pathways to design next-generation optoelectronic hardware and smart sensor arrays without relying on traditional toxic components. This paper presents an integrated computational informatics and experimental optimization approach for designing lead-free core/shell heterostructures as high-efficiency components for optical computing circuits, smart environmental sensors, and advanced display matrices. Density functional theory (DFT) simulations were deployed as a predictive modeling framework to analyze the electronic structure, energy band gaps, and stability parameters of the systems, thereby minimizing physical prototyping loops. Experimentally, a wider-bandgap semiconductor shell was epitaxially engineered onto the ternary core using an optimized high-temperature hot-injection protocol to passivate surface traps and stabilize functional electronic channels. Characterization via TEM, XRD, DLS, and photoluminescence spectroscopy confirmed that precise algorithmic control over synthesis kinetics increased the photoluminescence quantum yield from 5% to 65%. The engineered nanocrystals exhibited broad-band emission (550–750 nm), superior photostability, and an optimized average hydrodynamic size of 6.5 nm, preventing signal degradation in high-density device integration. A controllable redshift of the absorption edge from 495 to 583 nm was achieved by adjusting isothermal processing milestones, validating predictable bandgap tuning. The convergence of DFT computational informatics and controlled synthesis provides a robust methodology for the scalable production of non-toxic, highly stable optical hardware blocks tailored for IoT networks and green computing architectures.