We report a cost-effective way to synthesize the lithium silicate nano-glass ceramics for high-performance Li-ion batteries (LIBs). By proper heat treatment on the precursor glass, we succeeded in preparing Li2TiSiO5 glass ceramics, based on which the anode was fabricated. This type of anode exhibits superior electrochemical performances, that is, a specific capacity of about 180 mA h g−1 until 5000 cycles at 5 A g−1. This high cycling stability is attributed to the synergistic effect of both the open network in the glass matrix and the crack-type channels induced by Li2TiSiO5 nanocrystals in the glass matrix. The open network could withstand the volume change and the stress caused by Li+ insertion/extraction, while the nanocrystals could provide efficient pathways for fast ion delivery and electron transport. The present work has a promising potential to develop high-performance electrode materials for LIBs.