With the rapid growth of E-commerce business, logistics service, especially the last-mile distribution, has become one bottleneck, which leads to the rise of coordination complexity of logistics service supply chain (LSSC). This research, based on Stackelberg’s game theory, studies the coordination of a new three-echelon LSSC consisting of an E-commerce mall, an express company, and a terminal distribution service provider and investigates the optimal solutions and profits for each party within the semicentralized and centralized LSSC alliances, respectively. To accomplish this, it firstly shows that the three-echelon LSSC can lead to global optimum under the centralized decision-making scenario and then deploys the contract coordination schemes, including revenue sharing, cost sharing, and unit delivery price contracts, in three semicentralized alliances, so as to achieve the same performance of the centralized decision-making scenario, in which each party in the LSSC can achieve the win-win situation. Finally, numerical examples are provided to illustrate the feasibility and the effectiveness of the proposed coordination strategies. This study enriches the coordination theory in the field of LSSC and provides managerial insights for decision makers in LSSC.