Carbon-coated LiTi2(PO4)3 (LTP/C) nano- and/or microcrystals have been subjected to extensive research due to their potential application in aqueous rechargeable lithium-ion batteries (ARLBs) with enhanced electrochemical performance. In this paper, mesoporous LTP/C nanocrystals have been prepared by annealing the precursor obtained through a simple room-temperature co-precipitation method. The mesoporous LTP/C nanocrystals have been evaluated in the role of anode materials for lithium-ion batteries (LIBs) with organic and water electrolyte, respectively. After 1000 cycles at 5 and 20C, the specific discharge capacity of the LTP/C electrode with organic electrolyte retains 116.9 and 80.4mAhg−1, with capacity retention of 94.4% and 80.4%, respectively. After 1000 cycles at 1.37C, the specific discharge capacity of the LTP/C‖LiMn2O4 pouch cells with 1molL−1 Li2SO4 electrolyte retains 20.1mAhg−1, presenting a discharge voltage plateau around 1.21V and a capacity retention of 71.5%. The enhanced electrochemical performance of the mesoporous LTP/C nanocrystals makes them a promising candidate functioning as anode materials for LIBs and hybrid supercapacitors.