Electron–phonon interactions play a central role in determining the electrical, thermal, and optical properties of nanocrystalline solids. In reduced dimensions, quantum confinement, grain boundaries, and enhanced surface-tovolume ratios significantly modify both electronic states and lattice dynamics, leading to deviations from bulk behavior. This study investigates the nature of electron–phonon coupling in nanocrystalline materials through a combined experimental and theoretical approach. Structural and spectroscopic characterization, temperature-dependent electrical transport, and Raman spectroscopy were employed to probe phonon confinement and carrier–lattice coupling. The results demonstrate enhanced electron–phonon scattering in nanocrystalline systems, manifested as increased resistivity, phonon softening, and modified carrier relaxation dynamics. These findings highlight the critical role of nanoscale structural features in governing electron–phonon interactions and their implications for nanoscale electronic and thermoelectric devices.