Fe 3 O 4 nanoparticles (NPs) with an average size of 8-10 nm and a loading ratio of 50 wt% have been successfully attached onto the external surfaces of multi-walled carbon nanotubes (MWNTs) by means of three different preparative approaches, namely a sonication method, a covalent attachment protocol, as well as a non-covalent π-π interaction strategy. Specifically, the Fe 3 O 4 NPs associated with the sonication method lie directly on the outer surfaces of the MWNTs. Particles covalently attached onto the MWNTs formed amide chemical bonds through the mediation of the amorphous (3-aminopropyl) triethoxysilane (APTES) linker. Finally, particles were anchored non-covalently onto the underlying conjugated MWNTs via an aromatic 4-mercaptobenzoic acid (4-MBA) linker. Both structural and electrochemical characterization protocols have been used to systematically correlate the electrode performance with the corresponding attachment strategies. Fe 3 O 4 -MWNT composites generated by the π-π interaction strategy delivered 813, 768, 729, 796, 630, 580, 522, and 762 mAh/g under rates of 200, 400, 800, 100, 1200, 1600, 2000, and 100 mA/g, with 72% retention between cycles 2 and 80, demonstrating both higher capacity and better cycling stability as compared with analogues derived from the physical sonication as well as covalent attachment strategies. This finding may be attributed to the enhanced charge and ion transport coupled with retention of physical contact with the underlying MWNTs after a large volume change during cycling. Our collective results suggest that the non-covalent π-π attachment modality is a more effective preparative strategy for enhancing the performance of MWNT-Fe 3 O 4 composite electrodes after a full discharge process. Lithium ion battery (LIB) applications have experienced significant growth over the past two decades. Today LIBs are widely used and denote the battery of choice for a wide range of applications spanning from portable electronics to electric vehicles.1-5 Although LIBs have shown impressive commercial success, an understanding of the intrinsic functioning of LIB electrodes and of their constituent component materials still represents a subject of significant research. In recent years, the use of energy storage devices has expanded into new areas, including with uninterrupted power sources (UPS), stationary storage batteries (SSBs), and the automotive market, the latter of which encompasses both electric vehicles and hybrid electric vehicles. Hence, the development of LIBs based upon the use of lower cost and more earth abundant materials embodies a highly desirable objective.As an electroactive material, the inverse spinel structure of magnetite (Fe 3 O 4 ) epitomizes a particularly promising candidate for an anode material in LIB, due to its (i) significantly larger reversible capacity (i.e. 926 mAh g −1 , when reacting with eight lithium equivalents), (ii) plentiful earth abundance, and (iii) relative non-toxicity.