Transition metal chalcogenides (TMDCs) present an excellent initial discharge capacity for aluminum ion batteries (AIBs). However, its strong acting force with Al3+ and poor electrical conductivity hinder the further application of TMDCs in high-capacity AIBs. In this work, Peony-like MoSe1.48S0.52@C was prepared for AIBs cathode by hydrothermal method. The outsourced carbon reduces the agglomeration of MoSe1.48S0.52. Meanwhile, the S doping to form Se1.48S0.52 interlayer ligands, together with the Se presence to lower the band gap, enhances electrons transport and storage performance of aluminum. In addition, the material MoSe1.48S0.52@C can stably accommodate S nanoparticles and anchor aluminum sulfide to enhance the electrochemical stability of the cathode. The electrochemical test result shows that the specific capacitance of MoSe1.48S0.52@C reaches 300.8 mAh g−1 at 100 mA g−1. Note that the specific capacity for MoSe1.48S0.52@C@S is up to 1000 mAh g−1 at 200 mA g−1.