A high performance LiMnPO4/graphene nanocomposite as cathode material for lithium-ion batteries was prepared via surface modification of 3-aminopropyltrimethoxysilane (APS) on LiMnPO4 nanoparticles and electrostatic self-assembly of positively charged APS-LiMnPO4 nanoparticles and negatively charged graphene oxide. Successful APS modification on LiMnPO4 was demonstrated by the existence of 3-aminopropyl and Si-O-C groups in FTIR spectra. LiMnPO4 nanoparticles (ca. 25 nm) were found uniformly distributed on the surface of graphene sheets. The intimate contact of LiMnPO4 nanoparticles with graphene conductive network allows achieving fast electron transfer between the active material and charge collector and accommodating volume expansion/contraction of LiMnPO4 nanoparticles during electric discharge/charge process. The nanocomposite cathode material could deliver an initial capacity of 142.2 mA·h·g-1 at 0.05 C and maintain 90.5% capacity after 50 cycles
which were significant better than no APS-modified counterpart.