With a great potential to support multitudinous services and applications, mobile device-to-device (D2D) communications are conceived as a candidate paradigm for the future intelligent transportation systems and mobile Internet. To optimize the performance of underlaying mobile D2D communication systems with mutual interference caused by resource reuse, we propose two scenario-related power allocation schemes and investigate the energy efficiency (EE) and spectral efficiency (SE) trade-off. A 3-D vehicle-to-vehicle channel model is adopted to characterize propagation characteristics in realistic vehicular environments. We observe that a small degradation in EE around its peak value can significantly increase the SE for high vehicular traffic density (VTD) scenarios, while a marginal degradation in SE results in a considerable gain in EE for low VTD scenarios. Therefore, we maximize the SE subject to EE requirement in high VTD scenarios and maximize EE subject to SE requirement in low VTD scenarios. Moreover, to provide comprehensive understanding and further facilitate the practicality of EE-SE trade-off, economic efficiency (ECE) is employed as a general evaluation criterion to assess the efficacy of tradeoff. Finally, extensive simulations are provided to reveal the tradeoff quantitatively and demonstrate the viability that ECE can serve as a general metric for EE–SE trade–off in vehicular environments under different communication conditions.