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Ti3C2Tx MXenes modified with in situ grown carbon nanotubes (CNTs) are fabricated via a simple catalytic chemical vapor deposition (CVD) process. The as-prepared Ti3C2Tx/CNT nanocomposites show that one-dimensional (1D) carbon nanotubes are uniformly distributed in the interlayers of two-dimensional (2D) Ti3C2Tx MXene flakes. Compared with the pristine Ti3C2Tx MXenes, the hierarchical sandwich microstructure makes a contribution to the excellent electromagnetic wave absorption performance in the frequency range of 2–18 GHz, including higher absorption intensity (the minimum reflection coefficient reaches −52.9 dB, ∼99.999% absorption), broader effective absorption bandwidth (4.46 GHz), lower filler loading (35 wt%) and thinner thickness (only 1.55 mm). In addition, with the adjustment of thickness from 1.55 to 5 mm, the effective absorption bandwidth can reach up to 14.54 GHz (3.46–18 …