Traffic congestion often incurs environmental problems. One of the most effective ways to mitigate this is carpooling transportation, which substantially reduces automobile demands. Due to the popularization of smartphones and mobile applications, a carpool service can be conveniently accessed via the intelligent carpool system. In this system, the service optimization required to intelligently and adaptively distribute the carpool participant resources is called the carpool service problem (CSP). Several previous studies have examined viable and preliminary solutions to the CSP by using exact and metaheuristic optimization approaches. For CSP-solving, evolutionary computation (e.g., metaheuristics) is a more promising option in comparison to exact-type approaches. However, all the previous state-of-the-art approaches use pure optimization to solve the CSP. In this paper, we employ the framework of neuroevolution to propose the self-organizing map-based neuroevolution (SOMNE) solver by which the SOM-like network represents the abstract CSP solution and is well-trained by using neural learning and evolutionary mechanism. The experimental section of this paper investigates the comparisons and analyses of two objective functions of the CSP and demonstrates that the proposed SOMNE solver achieves superior results when compared against those the other approaches produce, especially in regard to the optimization of the primary objective functions of the CSP. Finally, the visual results of the SOM are illustrated to show the effectiveness and efficiency of the evolutionary neural learning process.