Electromagnetic wave absorbers constructed by reduced graphene oxide (rGO) and magnetic nanoparticles are extremely desirable for enhancing electromagnetic wave absorption performance due to the effective integration of the properties of dielectric and magnetic materials. However, the arrangement of graphene sheets and the growth of magnetic nanoparticles have always been challenging. Herein, an in-situ growth process has been used to successfully prepare accordion-like graphene with homogeneously distributed Fe nanoparticles in the confined structure via ion absorption and pyrolysis. The as-prepared Fe/layered rGO composites show excellent electromagnetic wave absorption performance with thin thickness, low filler loading, and broad effective absorption bandwidth (EAB). The minimum reflection loss of the composites achieves −54.6 dB with 20 wt% filler loading, and the tunable EAB reach 6.8 GHz (2.2 mm with 10 wt% filler loading) and 4.6 GHz (2.8 mm with 30 wt% filler loading), which can cover the entire Ku-band and X-band. The mechanism analysis indicates that the superior absorption performance is attributed to the multi-component loss mechanism, enhanced impedance matching degree and attenuation ability caused by the synergistic effect of layered rGO sheets and magnetic nanoparticles. This work opens up a new avenue for constructing accordion-like graphene-based composites as highly efficient electromagnetic wave absorbers.