Current study reports the synthesis and characterisation of a new magnetic-photocatalyst (CoFe2O4-TiO2) and tests its feasibility to be used as smart magnetically-recoverable nanomaterials in photodegradation of methylene blue (MB). The 3D urchin-like TiO2 microparticles are hydrothermally prepared and decorated with CoFe2O4 magnetic nanoparticles (NPs) through a co-precipitation method. The as-prepared CoFe2O4-3D TiO2 nanocomposites show enhancement in photodegradation of MB if compared to commercial rutile-phase TiO2 and pure urchin-like TiO2 (3D TiO2) microparticles. Such enhancement could be accredited to the lower recombination rate of photoexcited charge carriers of CoFe2O4-3D TiO2 nanocomposites. Furthermore, the CoFe2O4-3D TiO2 nanocomposite is magnetically-retrievable for sequential recyclability, and the results indicate that the nanocomposite shows a relatively consistent photocatalytic performance with negligible degradation. Thus, the current study would offer a potential route in the design and processing of a value-added photocatalyst nanocomposite that will contribute to the advancement of photocatalysis study.