Lithium Iron (II) Silicate, Li2FeSiO4, is a promising cathode material for Li-ion battery applications. Its carbon composite Li2FeSiO4/C was synthesized by a simple dry ball-milling process combined with high- temperature treatment, using citric acid as carbon source, and characterized by temperature-dependence. Powder X-ray diffraction shows that it crystallizes in a monoclinic structure with (P21/n) symmetry. 57Fe Mössbauer effect studies in the temperature range 16.5–298 K were carried out. The temperature dependence of the isomer shifts was used to estimate the effective vibrating mass, Meff, yielding a value of ~87 g mol−1 for Fe in the FeO42-- moiety. This is due to the significant covalency of the Fe-0 bond in the orthosilicate composite. The temperature dependence of the recoil-free fraction (spectral areas), when combined with the effective vibrating mass calculation, yields the “Mössbauer lattice temperature” of θM = 165 K Low temperatures reveals that paramagnetic Li2FeSiO4/C becomes antiferromagnetic at 16.5 K.