Lead-free piezoelectric ceramic/epoxy composites with ``0-3`` connectivity were prepared by cold-pressing with a temperature controlled curing method. A ceramic powder with a composition of (Na0.51K0.47Li0.02)(Nb0.8Ta0.2)O3 was synthesized by a conventional solid state reaction route. The dielectric and piezoelectric properties of ceramic/epoxy composites were characterized as a function of the volume fraction (φ) of piezoelectric ceramics, which was varied from 70 to 95vol%. The results indicated that the piezoelectric properties of composites were significantly affected by the volume fraction of ceramics. In terms of the piezoelectric properties, specimens showed the best performance at φ= 85vol%, resulting in the piezoelectric constant d33 of 39pC/N and the figure of merit as a piezoelectric energy harvester (d33·g33) of 1.24 pm2/N.