Meticulous design and morphological tuning at nano/micrometer have been the focal point to modulate and comprehensively understand the kinetics of electrochemical reactions, especially in lithium-ion batteries (LIBs). In this report, we demonstrate an elegant approach to fabricate spinel-cobalt oxide (Co3O4) with sheet, pellet, flower, and cube-like morphologies. When evaluated as anode materials in LIBs, the Co3O4 nanomaterials with 2D sheet-morphology demonstrates the best electrochemical performance compared to those of Co3O4 materials with pellets-, flowers- and cube-like morphologies. Galvanostatic charge/discharge study of Co3O4 nanomaterials with 2D sheet-morphology shows an initial discharge capacity of 1618.0 mAh g−1 and a discharge capacity of 587.0 mAh g−1 is achieved even after 60 cycles at 0.1 C rate with an impressive columbic efficiency of ∼99%. Importantly, the sheet-structured Co3O4 electrode delivers a discharge capacity of 444.0 mAh g−1 at a high current of 1.0 C and provides 275.0 mAh g−1 even after 400 cycles with ∼99.0% columbic efficiency suggesting high electrode stability. The enhanced electrochemical performance of Co3O4 nanomaterials with 2D sheet-morphology is attributed to improved electrode/electrode interface with nano-sized particles and better accommodation of strain during charge/discharge processes compared to other morphologies.