Metal sulfides have a highly promising potential as anode materials for next-generation lithium-ion batteries (LIBs) due to their environmental friendliness, abundant resources, and low-cost. Unfortunately, the implementation of such novel anodes is severely hindered by their low electronic conductivity and large volume expansion during the repetitive lithiation/delithiation process. Herein, we report a specifically designed anode structure to overcome these obstacles, that is, to incorporate MxSy (M = Ni, Zn, and Fe) with graphene nanosheets (GNS) and carbon nanotubes (CNTs) to form three-dimensional interconnected MxSy-graphene nanosheets-carbon nanotubes aerogels. Morphology and structure results confirm that MxSy particles were uniformly and closely attached on the 3D complex network structure of GNS-CNT. As a result, when used as anode materials for half and full LIBs, the MxSy-GNS-CNT aerogels exhibit remarkable high reversible capacities, ultra-long cycle life, and super high rate performance (For example, the NiS-GNS-CNT, ZnS-GNS-CNT, and FeS2-GNS-CNT aerogels could deliver high capacities of 735, 800, and 850 mAh g−1 after 100 cycles, respectively). Our results indicate that 3D interconnected MxSy-GNS-CNT aerogels are promising anode materials for the next generation LIBs with high-performance.