A novel "201" nanostructure composite consisting of two-dimensional MoS2 nanosheets, zero-dimensional Ni nanoparticles and one-dimensional carbon nanotubes (CNTs) was prepared successfully by a two-step method: Ni nanopaticles were deposited onto the surface of few-layer MoS2 nanosheets by a wet chemical method, followed by chemical vapor deposition growth of CNTs through the catalysis of Ni nanoparticles. The as-prepared 201-MoS2-Ni-CNTs composites exhibit remarkably enhanced microwave absorption performance compared to Ni-MoS2 or Ni-CNTs. The minimum reflection loss (RL) value of 201-MoS2-Ni-CNTs/wax composites with filler loading ratio of 30 wt % reached -50.08 dB at the thickness of 2.4 mm. The maximum effective microwave absorption bandwidth (RL< -10 dB) of 6.04 GHz was obtained at the thickness of 2.1 mm. The excellent absorption ability originates from appropriate impedance matching ratio, strong dielectric loss and large surface area, which are attributed to the "201" nanostructure. In addition, this method could be extended to other low-dimensional materials, proving to be an efficient and promising strategy for high microwave absorption performance.