The microwave absorbing material with appropriate impedance matching and excellent attenuation ability can be applied to resist electromagnetic radiation. In this work, carbon nanotubes were modified by titanium dioxide via the atomic layer deposition method, to prepare lightweight composites with high microwave absorption performance. The impedance matching and attenuation ability of titanium dioxide/carbon nanotube (TiO2/CNT) composites could be precisely controlled by adjusting the number of titanium dioxide deposition cycles. The relationship between the microstructure and microwave absorption performance of the composite was analyzed in detail. When the number of TiO2 deposition cycles was 100, the composite displayed outstanding microwave absorption performance, due to appropriate impedance matching and strong attenuation ability. The maximum effective absorption bandwidth of the composite reached 5.19 GHz (1.6 mm), which almost covered the Ku band. The microwave attenuation mechanism of the composite has also been investigated. This work provided a new idea for fabricating lightweight microwave absorption materials.