As a zero-strain anode for lithium-ion batteries, spinel Li4Ti5O12 has been extensively investigated and considered to be a potential alternative to the commercial graphite due to its good safety and superior structural stability. Nevertheless, the bad conductivity and slow Li-ion diffusion inhibit its scalable application. In this work, the 1D Li4Ti5O12 nanofibers are successfully fabricated by using an electrospinning method, and then the nanofibers are coated with the conductive PANI layer through an in-situ polymerization. The as-prepared Li4Ti5O12@PANI composite exhibits superior electrochemical performances such as high specific capacity, good rate property and excellent cycle stability. The excellent Li-storage properties can be attributed to the improved conductivity and effective Li-ion transportation of the composite. The results reveal that the Li4Ti5O12@PANI electrode is a good candidate for lithium-ion batteries. Meanwhile, this novel strategy presented here can be applicable for the fabrication of other electrode materials for electrochemical energy storage.