The strain-mediated magnetoelectric (ME) coupling between piezoelectric (PE) and magnetostrictive (MS) components are established in various connectivities. Discovering new ME connectivity and elucidating the key factors governing the performance of ME composite are of critical importance to find advanced materials for modern electronics. Reported here is a novel ME coupling in 0-1 connectivity. The unique self-assembling ability of 1-dimension crystalline nanocellulose (CNC) nanowhiskers enables the establishment of ME coupling with 0-dimension cobalt ferrite (CFO) nanoparticles without the use of binder. The developed CFO/CNC 0-1 ME composites display a significant ME voltage coefficient (αME) as high as 0.135 mV cm−1 Oe−1. The CFO nanoparticles are also modified with a cationic surfactant, cetyltrimethylammonium bromide (CTAB), to reduce their dispersion ability. A ME response related to the rearrangement of aggregated MS nanoparticles is observed in the CTAB-CFO/CNC composites, which differs from the typical magnetostriction induced ME effect in nanoparticulate ME composites.