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This paper reports the fabrication of novel hybrid and structured materials by using hemp fibers as organic support. Two in-situ methodologies were proposed and applied to modify the surface of hemp fibers in order to improve their physical properties and to confer a magnetic behavior: i) coprecipitation of Fe/Al layered double hydroxides through urea method (MHF@LDH Fe/Al) and ii) deposition of Fe 3 O 4 particles onto AlOOH modified hemp fibers in ammonia solution (MHF@AlOOH-FePs). The obtained hybrid materials have been widely characterized in terms of spectroscopic, morphological, thermal and barrier properties. Finally, a further investigation concerned the evaluation of surface charge and the estimation of magnetic properties showing a ferromagnetic behavior (Curie Temperature T c > 300 K) for both samples with a coercive field of H c ≈± 40 Oe for MHF@LDH Fe/Al and H c ≈ ± 10 Oe for MHF@AlOOH-FePs. [Display omitted] • Fabrication of novel hybrid materials based on hemp fibers and Fe/Al. • Two in-situ surface modification methodologies have been investigated. • Ferromagnetic behavior of Fe/Al-hemp based materials has been observed. [ABSTRACT FROM AUTHOR]