Direct attachment of MoS2 to materials with carbonaceous architecture remains a major challenge because of non-intimate contact between the carbonaceous materials and active MoS2 material. In this study, we report a new unique synthetic method to produce a new type of hybrid nanostructure of MoS2-CNTs composites. We developed a novel strategy for the synthesis of cylindrical MoS2 directly grown on CNT composites without the use of any other additives, exhibiting superior electrochemical performance as the anode material of lithium-ion batteries via a microwave irradiation technique. We adopted a simple step-by-step method: coating sulfur on CNTs and then reaction with a Mo source to synthesize hybrid cylindrical nanostructures of the MoS2-CNT composite. X-ray diffraction, field emission scanning electron microscopy, and high-resolution transmission electron microscopy analyses demonstrated that the as-synthesized MoS2-CNTs possessed a hybrid nanostructure, in which MoS2 sheets were well attached to the CNTs. The directly attached MoS2 sheets on the CNTs showed superior electrochemical performance as anode materials in a lithium-ion battery.