In order to achieve the goal of low-carbon, efficient delivery using unmanned vehicles, a multi-objective optimization model considering carbon emissions in the problem of optimizing multi-route delivery for unmanned vehicles is proposed. An improved genetic algorithm (IGA) is designed for solving this problem. This study takes into account constraints such as the maximum service duration for delivery, the number of vehicles, and the approved loading capacity of the vehicles, with the objective of minimizing the startup cost, transportation cost, fuel cost, and environmental cost in terms of the carbon dioxide emissions of unmanned vehicles. A combination encoding method based on the integer of the number of trips, the number of vehicles, and the number of customers is used. The inclusion of a simulated annealing algorithm and an elite selection strategy in the design of the IGA enhances the quality and efficiency of the algorithm. The international dataset Solomon RC 208 is used to verify the effectiveness of the model and the algorithm in small-, medium-, and large-scale cases by comparing them with the genetic algorithm (GA) and simulated annealing algorithm (SA). The research results show that the proposed model is applicable to the problem of optimizing the multi-route delivery of unmanned vehicles while considering carbon emissions. Compared with the GA and SA, the IGA demonstrates faster convergence speed and higher optimization efficiency. Additionally, as the problem’s scale increases, the average total cost deviation rate changes significantly, and better delivery solutions for unmanned vehicles are obtained with the IGA. Furthermore, the selection of delivery routes for unmanned vehicles primarily depends on their startup costs and transportation distance, and the choice of different vehicle types has an impact on delivery duration, total distance, and the average number of trips. The delivery strategy that considers carbon emissions shows a 22.6% difference in its total cost compared to the strategy that does not consider carbon emissions. The model and algorithms proposed in this study provide optimization solutions for achieving low-carbon and efficient delivery using unmanned vehicles, aiming to reduce their environmental impact and costs. They also contribute to the development and application of unmanned vehicle technology in the delivery field.