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Lithium-ion batteries (LIBs) have been explored to meet the current energy demands; however, the development of satisfactory anode materials is a bottleneck for the enhancement of the electrochemical performance of LIBs. Molybdenum trioxide (MoO3) is a promising anode material for lithium-ion batteries due to its high theoretical capacity of 1117 mAhg−1 along with low toxicity and cost; however, it suffers from low conductivity and volume expansion, which limits its implementation as the anode. These problems can be overcome by adopting several strategies such as carbon nanomaterial incorporation and polyaniline (PANI) coating. Co-precipitation method was used to synthesize α-MoO3, and multi-walled CNTs (MWCNTs) were introduced into the active material. Moreover, these materials were uniformly coated with PANI using in situ chemical polymerization. The electrochemical performance was evaluated by galvanostatic charge/discharge, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). XRD analysis revealed the presence of orthorhombic crystal phase in all the synthesized samples. MWCNTs enhanced the conductivity of the active material, reduced volume changes and increased contact area. MoO3-(CNT)12% exhibited high discharge capacities of 1382 mAhg−1 and 961 mAhg−1 at current densities of 50 mAg−1 and 100 mAg−1, respectively. Moreover, PANI coating enhanced cyclic stability, prevented side reactions and increased electronic/ionic transport. The good capacities due to MWCNTS and the good cyclic stability due to PANI make these materials appropriate for application as the anode in LIBs.