The relentless expansion of urban populations and the surge in e-commerce have increased the demand for rapid delivery services, leading to an increase in truck traffic that contributes to urban congestion, environmental pollution, and economic inefficiencies. The critical challenge this poses is not only in managing urban spaces efficiently but also in aligning with global sustainability goals. This study addresses the pressing need for innovative solutions to reduce reliance on truck transportation in congested urban areas without compromising the efficiency of freight delivery systems. This study contributes a novel approach that leverages electrified and autonomous aircraft (EAA) cargo shuttles to shift the bulk of air transportable freight from road to air, specifically targeting underutilized airports and establishing vertiports in remote locations. By applying data mining techniques to analyze freight flow data, this research identifies key commodity categories and metropolitan statistical areas (MSAs) where the implementation of EAA services could significantly mitigate truck-induced congestion. The findings reveal that targeting a select few commodities and MSAs can potentially decrease truck traffic, with electronics emerging as the dominant commodity category, and cities like Los Angeles and Chicago as prime candidates for initial EAA service deployment. Stakeholders in urban planning, transportation logistics, and environmental policy will find this study’s insights beneficial. This work lays a foundation for future innovations in sustainable urban mobility and logistics.