In this study, we presented the design and preparation of a double nano-carbon modified Li4Ti5O12 composite, where an amorphous carbon layer derived from thermal decomposition of stearic acid (SA) was coated on the surface of Li4Ti5O12, while decorated with carbon-nanotubes (CNTs) as conductive network. A series of Li4Ti5O12–SA/CNTs composite was prepared by changing the amount of added SA and CNTs, and the effects of their proportion on the electrochemical properties of the as-prepared composites were systematically investigated. It was found that when used as anode materials for lithium-ion batteries (LIBs), the Li4Ti5O12–CNTs/SA composite prepared by adding 0.4wt.% (mCNTs:mLi4Ti5O12) CNTs and 12wt.% (mSA:mLi4Ti5O12) SA showed the remarkably high discharge specific capacity of 215.8mAhg−1 and the capacity retention reached as high as 96.7% with delivering a stable capacity of 145.0mAhg−1 after 100 cycles at the rate of 5C. Our work revealed that there is a cooperative effect resulted from adding proper proportion of CNTs and SA, enabling significant improvement of the electrochemical performances of Li4Ti5O12 as anode for LIBs.