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The self-assembled synthesis of a hierarchical graphene oxide (GO)-carbon nanotubes (CNTs)-α-FeOOH decorated composite aerogel (α-FeOOH@GCA) through a facile in-situ hydrolysis route is reported for the first time and the materials was tested for its performance as Fenton-like catalyst. The introduction of GO-CNTs clearly mediated the morphology to aligned α-FeOOH nanorods (ca. 100 nm) within aerogel matrix comparing with pristine urchin-like α-FeOOH three-dimensional microstructures (ca. 1 μm). This three dimensional porous aerogel network provided efficient charge/mass-transfer leading to great enhancement of the catalytic activity of α-FeOOH. The outstanding catalytic performance of this composite in degradation of organics with different charge and structure, i.e. Orange II (OII), rhodamine B (RhB), methylene blue (MB), phenol and endocrine disruptor bisphenol A (BPA) was demonstrated. For …